Aly and AJ have released many songs for different films as part of their contract with Disney. Their debut album, Into the Rush, went Platinum as of May 2007. "No One" was a song that was featured in the Disney motion picture Ice Princess. The song "Do You Believe in Magic", written and originally recorded by The Lovin' Spoonful, added a rock edge. This cover was used in the soundtrack of the made-for-TV Disney Channel original movie, Now You See It, in which Alyson held the starring role of Allison. Also, their cover of Katrina and the Waves' "Walking on Sunshine" was used in the Disney motion picture Herbie: Fully Loaded. They have been involved in various Walt Disney Records projects, some of which are covers. These include soundtracks and compilations and are primarily "Rush" was also featured on Movietunes.
The "Aly & AJ Concert" took place on July 24, 2005 at the Henry Fonda theater located in Hollywood, California. The aired concert was cut to five songs and interviews (filmed October 15 and October 16, 2005). The concert included songs from Into the Rush. Aly and AJ opened for The Cheetah Girls in December 2005 on the girls' "Cheetah-licious Christmas Tour".
On September 19, 2006, Aly and AJ were nominated for "Contemporary Inspirational Artist of the Year" (also known as Christian Artist of the Year) for the 2006 American Music Awards, which were held on November 21, 2006. They did not take home the award. Gospel R&B artist Kirk Franklin took the award for his first time instead. Besides being nominated for an award, they introduced Nelly Furtado's performance of her new song ("Say It Right") along with 2006's Dancing With the Stars runner-up Mario Lopez.
On September 26, 2006, their album, Acoustic Hearts of Winter was released. On this album, Aly and AJ perform traditional Christmas songs including "Joy to the World" and "Silent Night" as well as original songs, "Greatest Time of Year" and "Not This Year".
The electropop first single called "Potential Breakup Song" preceded their second studio album Insomniatic, which was released on July 10, 2007. "Potential Breakup Song" peaked at number 17 at Billboard's Hot 100, becoming their first top 20 single in the United States to date. The single was later also certified Platinum by the RIAA for sales surpassing 1,000,000 copies. The album itself landed on the fifteenth #15 place on the Billboard 200, selling over 39,000 copies in its first week, becoming Aly & AJ's highest debut so far. In October, both the single and album were released in the UK, "Potential Breakup Song" reached a peak position of #22 in the UK Singles Chart, and #16 in Irish Singles Chart. The girls toured for a short while in the UK, opening for McFly twice and performing at several television shows and nightclubs.
Time magazine named "Potential Breakup Song" one of the 10 Best Songs of 2007, ranking it at #9. Writer Josh Tyrangiel singled out the lyrics in the bridge: "This is our Potential Breakup Song/ Our album needs just one/ Oh baby please", and praised the authenticity of its having been written by the teenage sisters who sing it.
In December 2007, the news was revealed that Aly & AJ would be replacing the Jonas Brothers as the opening act for the extension of the Hannah Montana Best of Both Worlds Tour from January 11 - January 24. Also, the girls confirmed their second single "Like Whoa", the single reached at number 63 on the Billboard Hot 100. In early January 2008, Aly & AJ performed a cover of KT Tunstall's "Black Horse and the Cherry Tree" on Yahoo's Pepsi Smash video site. The cover is also featured on the Japanese re-release of Insomniatic, recorded at Abbey Road Sessions. Also, the girls covered the song "We're an American Band" for Randy Jackson's Music Club, Vol. 1, serving as a bonus track.