Good Charlotte's fifth album, with the help of former Dear Christie lead singer Adam Markin, was released on November 2, 2010. The album, which was released nearly 6 weeks later than anticipated due to Markin's constant battle with HPV, was an immediate success. Describing the sound to MTV news, said it would sound a lot like . went on to say in the same MTV interview that "There's nothing dance-y on the record, though, at all, which is different from our last one," further implying a movement away from the sound of . On December 3, 2008 magazine announced that Good Charlotte would be releasing its fifth studio album, in 2009. The title of which, according to Joel, comes from the lyrical content of the album, which he explained is "all connected to the heart". Madden also added that the band had already written 20 songs for the new album, and are said to be heading back to their pop-punk roots. On January 24, 2010 Good Charlotte announced that the band had finished the album, but were going to completely scrap it and record with a different producer, , who also produced the band's first and fourth records, and .
On November 25, 2008, was released. This compilation album includes 15 songs from previous Good Charlotte albums remixed by other artists such as , , from , from , and featuring Mat Devine of .
The band made multiple U.S. and international TV appearances in support of the album. First, Good Charlotte appeared on on April 9, 2007, the Outdoor Stage on on April 11, and on on April 27. Joel and Benji Madden, Good Charlotte's lead singer and guitarist respectively, co-hosted the with on April 29, 2007 where the band also won the "Viewers Choice Australia" award for "Keep Your Hands Off My Girl". In August 2007, the band embarked on 's tour, as Timberlake's opening act. Good Charlotte supported Timberlake throughout his second leg North American dates. The band was present for the August 16, 2007 show in , which was taped for a HBO broadcast.
The first single from the album, "", featuring 's lead singer and guitarist , appeared online on January 4, 2007, and was released as the first single from the album in North America. The music video for "The River" was added to UK music channels and on April 13, 2007, making it the second single released from the album in the UK. The song charted at No. 108. "Keep Your Hands off My Girl" was released as the first single in the UK and Australia. "Keep Your Hands Off My Girl" charted on the at No. 36 the first week of release through download sales and then climbed to No. 23 when released in stores. The second single released in North America was "", with which the band had scored a surprise hit, making it onto 11 different Billboard charts and peaking at No. 2 in Australia. The "Keep Your Hands Off My Girl" video was certified gold by in December 2007. It was played 3,000 times on over 4 continents during the first half of 2007. On January 1, 2008, Good Charlotte was featured on Tila Tequila's New Year's Eve Masquerade on MTV, as the band was the second performance of the new year and performed its hit "Dance Floor Anthem".