Ali signed for Warwickshire aged just 15, hitting a half-century for the county’s Second XI a few days before his 16th birthday. After more games at this level in 2004, and a first outing for England Under-19s against their Bangladeshi counterparts he spent the succeeding winter playing for the Under-19s on their tour of India.

2005 saw Ali make his first-class debut, against Cambridge University in May. He impressed with the bat, making 57 not out in his only innings, and sent down two overs for 15 runs. Playing that summer against Sri Lankan Under-19s, he starred in the final “Test” by making 52 not out and 100 not out (the latter innings from 56 balls) and claiming seven wickets. He was then selected for the 2006 Under-19 Cricket World Cup, which was held in Sri Lanka, and was immediately promoted to captain by coach Andy Pick. He made three half-centuries in the tournament, and took seven wickets.

Ali received additional opportunities for his county in 2006, playing his first List A games. The first of these came against Derbyshire, where he dismissed Steffan Jones to claim his maiden first-team wicket. He also took his first wickets in first-class cricket, and his first three victims were all Test players: Stuart Law, Dominic Cork and Dave Mohammed. With the bat he scored 68 on his County Championship debut against Nottinghamshire, then equalled that score against Durham.

Ali’s opportunities were somewhat limited, however, and Alex Loudon took his place in the side. In July 2006, with the expiry of his Warwickshire contract only months away, Ali brushed off rumours of a move to Worcestershire, saying “I don’t know anything about it”, but in September it was announced that Ali would indeed be leaving to join that county. The player himself said that he had been impressed by Worcestershire and felt it gave him the best prospects of furthering his career.

He made his debut for Worcestershire in their ten-wicket win over Loughborough UCCE on 25 April 2007.

At the end of the 2010 season Worcestershire secured promotion to the first division of the County Championship. After he was overlooked by the England Lions and England Performance Programme at the end of the 2010 English season, Moeen opted to play club cricket in Bangladesh at the suggestion of Bangladesh all-rounder Shakib Al Hasan. Shakib played for Worcestershire as their overseas player in 2010 and the link with the club led to Moeen representing Mohammedan Sporting Club in the Ispahani Premier Division.

During the 2011 season, Moeen spent three weeks as Worcestershire’s acting captain while the usual club captain, Daryl Mitchell, was injured. Though he had captained England Under-19s, it was the first time he filled the role for his county. As he was inexperienced, Moeen approached senior players Vikram Solanki and Ben Scott for advice.

Pakistan off-spinner Saeed Ajmal was Worcestershire’s overseas player for a short time in 2011 and while at the club he encouraged Moeen to try bowling the doosra. Moeen had to wait until July before registering his first century of the season, and his first since September the previous year. His innings of 158 runs from 244 balls against Somerset was in vain as Worcestershire succumbed to an innings defeat. The following month Moeen twice scored a century in the Clydesdale Bank 40 only for Worcestershire to lose, against Sussex and the Netherlands. In the first match against Sussex he passed his previous best score of 136 in List A cricket, scoring 158 runs from 92 balls. In Worcestershire’s first season back in the first division, Moeen scored 930 runs in the County Championship, making him the club’s second-highest run scorer in the competition behind Solanki. Moeen average 33.21 runs per innings and scored a single century. On the back of his performances for Worcestershire, Moeen was included in the 13-man England Development squad which trained in late 2011.

In February 2012, before the start of the English season, Worcestershire’s director of cricket Steve Rhodes commented that Ali’s doosra was “not too difficult to pick at the moment but he’s learning a few tricks and he’s got other things up his sleeve. It’s a work in progress”.

Ali was included in the English Squad for the 2014 ICC World Twenty20 in Bangladesh. Before the tournament, the squad played the West Indies in a limited overs series, and Ali made his ODI debut against the West Indies on 28 February 2014. He scored 44 runs before being dismissed and took his maiden ODI wicket. In the second match he made ten runs and took figures of 1–11. Ali was again impressive in the third match, making his first half century in a score of 55. He ended up scoring 109 runs and picking up 3 wickets in the three match series. He made his T20 debut in the second match of the T20 series, although he scored just 3 runs and did not bowl.

In the first Test against Pakistan in 2015, Ali struggled with the ball, conceding 121 runs in the first innings without taking a wicket, although he did take two wickets in the second innings. In his new role as opener, he made 35 with the bat in the first innings and 11 in the second as the match ended in a draw. In the first innings of the second Test, he took figures of 3–108, but again struggled with the bat, making scores of 1 in both innings as England slumped to defeat. He took 2–49 in Pakistan’s first innings as they were dismissed for 234 in the third Test, although he only scored 36 runs in the match as England lost by 127 runs.

Ali is an Ambassador of StreetChance, a programme providing free weekly cricket coaching sessions in deprived areas in the UK, run by the Cricket Foundation and Barclays Spaces For Sports. In January 2015, he joined Orphans in Need, an international NGO, as a Global Brand Ambassador and carried the charity’s logo on his bat. Speaking after his stint at the crease, Moeen Ali said, “I enjoy coming back to the community where I grew up playing tapeball cricket. It keeps you grounded. I hope that, as an ambassador for the charity, I can pass on some useful advice and help inspire children like the ones here today involved in StreetChance. It’s so important that schemes like StreetChance give young people the opportunity to play cricket and to learn key life skills, wherever they’re from, whatever their background.”

In January 2015, Ali was nominated for the Best at Sport award at the British Muslim Awards.

In April 2019, he was named in England’s squad for the 2019 Cricket World Cup. On 21 June 2019, in the match against Sri Lanka, Ali played in his 100th ODI.

In August 2019, Ali played against Australia in the first test match held as part of the 2019 Ashes series. Following England’s defeat, Ali was dropped by England for their second Test match. Ali subsequently announced that he would be taking a “short break” from cricket. On 29 May 2020, Ali was named in a 55-man group of players to begin training ahead of international fixtures starting in England following the COVID-19 pandemic. On 17 June 2020, Ali was included in England’s 30-man squad to start training behind closed doors for the Test series against the West Indies. On 9 July 2020, Ali was included in England’s 24-man squad to start training behind closed doors for the ODI series against Ireland. On 21 July 2020, the ECB named Moeen Ali as England’s vice-captain for the ODI series.

In December 2019, he was drafted by Multan Sultans as their Platinum Category pick at the 2020 PSL Draft.

On 8th September 2020, Moeen first captained England in a T20I match against Australia in Southampton. He became the first Asian-origin cricketer to captain England in T20s, and the first Asian-origin cricketer to captain England in any format since Nasser Hussain in 2003.