While at Le Havre, Payet endured a tumultuous four years. While training at the club, he was accused of having a difficult character and displaying a lack of motivation. The accusations ultimately led to his departure in 2003 as Payet returned to Réunion to sign with AS Excelsior. He spent only a year and a half at Excelsior playing in the Réunion Premier League before being signed in January 2005 by Nantes who sought to give the player another opportunity to prove himself on the mainland. Payet signed a two-year amateur deal with the club; however, Nantes were given the option of terminating the contract after six months.

Upon his arrival at Nantes, Payet was inserted onto the club’s reserve team in the Championnat de France amateur, the fourth level of football in France. In the 2005–06 season, Payet quickly established himself as one of the best players on the reserve team. He impressed with the team in 22 matches scoring six goals and was described by the club’s reserve team coach Stéphane Moreau as a “talented player despite his natural indifference”. His influential play with the team resulted in the player being called up to the senior team in December 2005 by manager Serge Le Dizet. Payet made his professional debut on 19 December in a league match against Bordeaux appearing as a substitute in a 0–0 draw. After the winter break, Payet remained with the senior team and scored his first professional goal in a 4–1 win over Metz. The midfielder appeared as a substitute in the match and had been on the field for no more than two minutes before netting the goal. After appearing in a league match against Toulouse on 4 February, Payet was relegated back to the reserve team for the rest of the season.

Ahead of the 2006–07 season, Payet signed a three-year professional contract with Nantes. He was officially promoted to the senior team and assigned the number 31 shirt by Le Dizet. After appearing as a substitute in the first two matches of the season, Payet made his first professional start on 9 September 2006 in a league match against Lille. In the match, he scored the equalizing goal in a 1–1 draw. Two weeks later, Payet started again and scored the opening goal in a 2–1 win against Marseille. Payet, subsequently, appeared as a starter for the rest of the campaign. He scored his only other goal during the season in a 1–1 draw with Sedan. One dark spot during the campaign was a straight red card in an embarrassing 5–2 loss to Valenciennes. Despite the successful individual season by Payet, Nantes ultimately finished the season in 19th place and were relegated, which meant the club would play in Ligue 2 for the first time since 1963.

In his first season at Saint-Étienne, Payet struggled to assert himself into the team. He made his club debut on 4 August 2007 in a 1–1 draw with Monaco. Despite being a starter for the majority of the campaign, Payet scored no goals and also failed to provide any assists. In a reversal of fortune, despite Payet’s sub-par season, Saint-Étienne finished in fifth place, which meant qualification to the UEFA Cup. In the 2008–09 season, Payet return to the form that resulted in Saint-Étienne signing the player. Prior to the start of the season, he was given the honour of captaining Saint-Étienne in a friendly match against the Réunion national team in the player’s return to the island. Payet appeared in 30 league matches scoring four goals and supplying six assists in the season. He scored his first league goal for the club on 29 September 2008 in a 1–1 draw with Bordeaux, netting the opener. In December 2008, he scored the game-winning goal against his former club Le Havre.

Payet is a former French under-21 international. He made his debut for the team in February 2007 in a friendly match against Switzerland, and assisted a Jérémy Ménez goal. In the team’s ensuing match against Denmark, he scored a double in a 3–1 win.

Payet featured in European competition for the first time after playing in the 2008–09 edition of the UEFA Cup. He made his debut in the competition on 18 September in the first leg of the team’s first round tie against Israeli club Hapoel Tel Aviv. On his debut, he scored the opening goal in a 2–1 win. In the group stage, Payet scored a goal in a 3–1 win over Danish club Copenhagen. In the knockout rounds, Payet was instrumental to the team’s 5–2 aggregate victory over Greek club Olympiacos. In the first leg, he assisted on a goal in a 3–1 win, while in the second leg, he netted the opener in 2–1 positive result. Saint-Étienne were eliminated from the competition in the next round by German club Werder Bremen, losing 3–2 on aggregate. Payet appeared as a substitute in both legs. Due to focusing its efforts on performing well in four competitions, Saint-Étienne finished one spot short of relegation in the league. On 22 July 2009, Payet signed a two-year contract extension with the club until 2013.

In the 2009–10 season, Payet remained consistent appearing in 35 league matches scoring two goals and providing six assists. He also performed well in the cup competitions, particularly in the Coupe de France. On 24 January 2010, he scored a double in 4–1 victory over Lorient. Two weeks later, he scored the winner against Vannes. Saint-Étienne ultimately reached the quarter-finals losing to Lens. On 18 May 2010, Payet was involved in a physical altercation with teammate and captain Blaise Matuidi during the team’s 1–0 defeat to Toulouse. Midway through the first half, Payet received criticism from teammate Yohan Benalouane for displaying a lack of aggression. He was then confronted by Matuidi, who echoed Benalouane’s sentiments. Payet and Matuidi suddenly went face-to-face with the former player delivering a blow to Matuidi’s head before the two were separated by referee Bruno Coue and teammates. As a result of the incident, Payet was substituted out after 31 minutes and sanctioned by club president Roland Romeyer. Payet apologized for the incident shortly after. On 6 October 2010, following both Payet and Matuidi’s call up to the national team, Payet described the incident as “an argument that had no place” and that “the incident was explained and the two were on new ground.” Matuidi described the altercation as a “lack of maturity” on both players part.

After the summer, Payet put the past behind him and opened the 2010–11 season by scoring seven goals in the first two months of domestic play. On 7 August 2010, he scored in the team’s opening 3–1 defeat to Paris Saint-Germain. On 29 August 2010, Payet scored his first professional hat-trick in a 3–1 victory over Lens. After the international break, he scored a double against Montpellier. On 25 September, Payet delivered a perfect free-kick goal in the team’s Derby du Rhône match against Lyon. The free-kick, described by local media as “superb and untouchable,” was the only goal in the team’s upset victory. The win placed Saint-Étienne in first place for the week. For his performances, Payet was awarded the UNFP Player of the Month award for September. Due to his performances domestically and international, Payet drew interest from several clubs, notably English clubs Chelsea and Liverpool. In January 2011, he was linked with a move to Paris Saint-Germain as the Parisian club looked to immediately replace the departed Stéphane Sessègnon. Payet sought for the move, but Saint-Étienne refused. Ahead of the closure of the transfer window, a frustrated Payet failed to show up to training in an effort to force the transfer. After returning to the team days later, Payet was demoted to the club’s reserve team ahead of the team’s league match against Montpellier on 5 February 2011.

Payet was called up to the senior national team for the first time by Laurent Blanc for the Euro 2012 qualifying matches against Romania and Luxembourg. He made his debut in the former on 9 October 2010, coming on as a substitute for Karim Benzema in the 86th minute and assisted Yoann Gourcuff’s goal to make it 2–0. Three days later, he came on for the last 30 minutes against Luxembourg and again assisted Gourcuff for a goal.

On 28 June 2011, Saint-Étienne manager Christophe Galtier confirmed that Payet was on the verge of signing with the defending league champions Lille after the player himself informed him the previous day. Hours later, the move was confirmed by both Saint-Étienne and Lille. Payet agreed to a four-year contract, while the transfer fee was priced at €9 million with future incentives to be included later.

Payet debuted for Lille in a 5–4 Trophée des Champions loss to Marseille at the Grand Stade de Tanger in Morocco on 27 July 2011. His Ligue 1 debut for the club came in the 2011–12 season opener against Nancy on 6 August. On 15 October, Payet scored his first goal for the club in a 3–1 win at Auxerre. Three days later, Payet made his UEFA Champions League debut as a 62nd-minute substitute for Benoît Pedretti in Lille’s 1–0 home loss to Italian club Internazionale.

On 18 May 2013, Payet was named in the UNFP’s Ligue 1 team of the season. He ended the season as the league’s joint-top assist-maker, alongside Mathieu Valbuena, with 12 goals created. He also scored 12 league goals to register the second-highest scoring season of his career.

On 27 June 2013, Marseille signed Payet for a fee in the region of €11 million. On his debut, he scored a brace within the first 15 minutes of the game, helping his side to a 3–1 victory over newcomers Guingamp at the Stade du Roudourou on 11 August.

In his second and final season with Marseille, Payet made more successful through-balls than any other player, with the exception of Lionel Messi, in European football’s top five leagues. He made almost twice as many key passes as any other player, and made 17 assists in 36 league appearances, topping the Ligue 1 assist charts. Payet credited his excellent 2014–2015 Marseille season which transformed his career to Marcelo Bielsa, who was appointed the head coach of Marseille on a two-year contract in May 2014. I clicked with him,” he later told L’Équipe. “He made me more mature and consistent. He put order into my game. I still have his advice in my head.” The key, according to Jan Van Winckel (who was Bielsa’s assistant during the 2014–2015 season), was giving him the pivotal No. 10 role and making him the focal point of attacks.

On 17 May 2015, he was named in the Ligue 1 team of the season by the UNFP for the second time.

On 26 June 2015, Payet joined Premier League club West Ham United on a five-year contract, with the option for an extra 12 months. The transfer fee West Ham paid to Marseille was reported to be £10.7 million. Payet had not intended to leave Marseille in the summer of 2015. Rather, his sale was subject to Marseille’s concern with financial stability after the sale of players such as Florian Thauvin and Giannelli Imbula had stalled. On 9 August, he made his Premier League debut against Arsenal at the Emirates Stadium and provided the free kick assist for Cheikhou Kouyaté to head in the opening goal of a 2–0 win. Six days later, he scored his first goal for the team, albeit in a 1–2 home defeat to Leicester City. Payet scored twice against Newcastle in a 2–0 win at the Boleyn Ground on 14 September. On 9 November, he was ruled out with an injury for an estimated three months after damaging his ankle in a tough challenge from Everton’s James McCarthy in a 1–1 home draw on 7 November. He scored his first goal from his return from injury in a 3–1 comeback win against AFC Bournemouth on 12 January 2016, equalising with a curling hit free-kick that went in off the underside of the crossbar, which was praised by several pundits. His Man of the Match performance received a standing ovation from West Ham fans as he was substituted in the 78th minute for Alex Song.

Payet scored his first goal on 7 June 2015, coming on for Mathieu Valbuena in the 73rd minute to net France’s third goal 16 minutes later, in a 4–3 home friendly defeat by Belgium. Six days later, Payet was substituted at half-time in a 1–0 away friendly defeat by Albania. Having been absent from the French squad since then, Payet was recalled in March 2016 for a squad to play the Netherlands and Russia. His performance on 25 March in a 3–2 win against the Netherlands in Amsterdam was praised by manager Didier Deschamps. Payet hit the post with a second-half shot and created six chances, more than double any other player. He also had the most touches of any player, with 89. Four days later, with his first touch after replacing Antoine Griezmann, he scored a 30-yard free kick against Russia and later assisted Kingsley Coman to confirm a 4–2 win.

In February 2016, Payet signed a new five-and-a-half-year contract with West Ham that would pay him £125,000 a week, committing him to the club until the summer of 2021. That March, Payet was named the Premier League Player of the Year at the 2016 London Football Awards. On 13 March, he scored a free kick, described by some journalists as “sublime” and “spectacular”, from 35 yards (32 m) as West Ham drew 1–1 at Old Trafford against Manchester United in an FA Cup quarter-final.

Following an outstanding first season in English football, Payet was named Premier League Player of the Year at the London Football Awards in March and shortlisted by the Premier League for the 2016 PFA Players’ Player of the Year Award. In May 2016, Payet became the 38th recipient of the West Ham United Player of the Year award.

In May 2016, Payet was named in the France squad for Euro 2016. He was named the Man of the Match for scoring a goal, laying on an assist, creating eight scoring chances and delivering 13 crosses in the opening match of Euro 2016, on 10 June, a 2–1 win for France against Romania. In that match, Olivier Giroud headed Payet’s cross into the goal in the 57th minute and Payet scored France’s second goal in the 89th minute — a curling and powerful left-footed shot into the top corner from 2 metres (2.2 yd) outside the penalty box. In France’s second group match against Albania on 15 June, Payet was again named the Man of the Match for creating six scoring chances for his teammates and supplying 17 crosses. In that match, Payet scored the second goal for France in a 2–0 win, the goal coming in the 96th minute. On 3 July, he scored and assisted in a 5–2 quarter-final win over Iceland at the Stade de France, as the hosts advanced to the semi-finals of the tournament. In the final of the tournament on 10 July, Payet was involved in a collision with Cristiano Ronaldo while attempting to challenge him for the ball, which resulted in an injury to the Portuguese forward and forced him off after 25 minutes of play. Payet was later substituted and Portugal eventually won the match 1–0 in extra time to lift the trophy.

On 12 January 2017, West Ham United manager Slaven Bilić announced that Payet no longer wanted to play for the club. He then did not feature at all in the matchday squad on 14 January, despite no reported injuries. At the London Stadium on that matchday, a mural installed in tribute to Payet winning Player of the Year was guarded by security in order to “prevent it being vandalised”. Payet was subsequently the subject of two bids from his previous club Marseille which were both rejected by West Ham. They stated that they did not want to sell the player, but would prefer him to apologise to fans and continue playing for the club. On 29 January, West Ham accepted an offer of £25 million from Marseille for the transfer of Payet, marking a club record sale for West Ham. The day after Payet completed his move to Marseille, his mural at the London Stadium was removed and replaced with one to commemorate Andy Carroll’s bicycle kick goal against Crystal Palace scored earlier in the month.

Payet made his second Marseille début in a 2016–17 Coupe de France clash with Olympique Lyonnais on 31 January 2017, appearing as a substitute in extra time at the Stade Vélodrome as his new club won 2–1. On 8 February, Payet scored his first goal since returning to OM in a 2–0 home victory over Guingamp.

On 3 May 2018, he played in the Europa League semi-finals away to FC Red Bull Salzburg as Marseilles played out a 1–2 away loss but a 3–2 aggregate win to secure a place in the 2018 UEFA Europa League Final. During the UEFA Europa League Final, Payet suffered an injury and was substituted on the 31st minute of the first half. Atletico Madrid beat Marseille 3–0.

On 10 August 2018, during a 4–0 victory for Marseille over Toulouse, Payet scored the first two goals of the 2018–19 Ligue 1 season, the second of which a converted penalty awarded using video assistant refereeing (VAR) technology; the first usage of VAR in French football.

During the COVID-19 pandemic in 2020, Payet’s club, Marseille were badly affected financially due to the cancellation of the 2019–20 season. As a result, several players accepted pay cuts in May 2020. Payet, the club’s top earner, refused such a cut as he had a family to support. In August 2020, Payet was one of five Marseille players who returned a positive test for COVID-19.