While attending Wellington High School in Wellington, Florida, Pope formed the band Blake with good friend Mike Gentile. The project disbanded before being signed and in 2008, she and Gentile along with Alex Lipshaw, Michael “Jersey” Moriarty, and Elliot James founded the pop punk band Hey Monday. Hey Monday released their first studio album, Hold on Tight, in October 2008. Pope wrote two songs and co-wrote the other nine songs. She appeared in Fall Out Boy’s video for “America’s Suitehearts”, from their 2008 album Folie à Deux. She also provided guest vocals for The Cab’s remix version of their song “Take My Hand” that appeared on Fall Out Boy’s mixtape, Welcome to the New Administration, and appeared in the music video for it the following summer of 2009. James left the band at the end of 2009. Hey Monday’s first EP Beneath It All was to be released in August 2010; to promote the album the group toured the US and played on the 2010 Warped Tour. The Christmas EP was released on December 6, 2011, and later that month Hey Monday took an indefinite hiatus on good terms.

In January and February 2012, Pope embarked on her first solo acoustic tour across the east and west coasts of the United States. She released her debut self-titled EP (self-labeled) on May 22, 2012, containing four songs written by Pope. She auditioned for season 3 of the singing competition The Voice during the summer and had all four coaches offer her a place on their teams; she ultimately picked country singer Blake Shelton. In the third live round, Pope performed “Over You”, co-written by mentor Shelton. The song reached number one on the iTunes chart, knocking Psy’s “Gangnam Style” down to number two. She was the only female contestant to advance to the Top 4 round where she performed “Stupid Boy” by country singer-songwriter Sarah Buxton, which also reached number one on iTunes. She advanced to The Voice finals, winning the title on the live finale results day in December. An album compiling her performances on The Voice entitled The Voice: The Complete Season 3 Collection reached No. 1 on the Heatseekers and sold 11,000 copies, and 8,000 more copies in the following week. Her self-titled EP also re-entered the chart at No. 42, selling 1,000 copies.

In January 2013, Pope signed with country music label Republic Nashville; the lead single of her solo album, “Wasting All These Tears”, was released on May 31, 2013. It debuted at number 37 on the Billboard Hot 100 and number 7 on the Billboard Hot Country Songs chart. It sold 125,000 copies in first week of release. The album, Frame by Frame, was released in October 2013. Pope spent most of 2014 touring with country artists Tim McGraw and Dierks Bentley. She also was featured on the Nashville Outlaws: A Tribute to Mötley Crüe album where she covered The Animal In Me.

Pope released the lead single, “I Am Invincible” from her upcoming second studio album. During late 2015, Pope recorded a duet with Chris Young, titled “Think of You” for his 2015 album I’m Comin’ Over. This single became Pope’s first song to peak at number one on the US Country Airplay chart in May 2016. In March 2017, Pope traveled to London and performed several times as part of the C2C: Country to Country festival line-up, including an appearance on the main stage with Young.

Pope’s new EP, Summer, was released on June 3, 2016 and the title track was released as a single on June 6, 2016.

On July 24, 2016, Pope sang the Star Spangled Banner, the United States national anthem, before the Brickyard 400 NASCAR race at the Indianapolis Motor Speedway.

On October 16, 2016, Pope sang the Star Spangled Banner, the United States national anthem, before the Houston Texans and Colts game.

In January of 2010, Pope began dating drummer Rian Dawson, who is a member of the band All Time Low. They became engaged in February of 2017. In July 2017, it was announced that the couple had ended their relationship.

On March 30, 2018 she independently released her first single in nearly 2 years, called “Take You Home”. It was followed on August 10 by her second single of 2018, called “One More Red Light”.

On February 1, 2019, Pope released her second full-length studio album, Stages.