The album was ranked #229 on Rolling Stone's list of The 500 Greatest Albums of All Time. The album's title track and Run–D.M.C.'s version of "Walk This Way" are part of The Rock and Roll Hall of Fame's 500 Songs that Shaped Rock and Roll list.
For Aerosmith's previous album, 1974's Get Your Wings, the band began working with record producer Jack Douglas, who co-produced the album with Ray Colcord. In the liner notes to the 1993 reissue of Greatest Hits it was said by an unnamed member of the group that they "nailed" the album. At the beginning of 1975 the band started working at The Record Plant in New York City for the album that became Toys in the Attic. The sessions for Toys were produced by Douglas without Colcord - the album was engineered by Jay Messina with assistant engineers Rod O'Brien, Corky Stasiak and Dave Thoener. The songs for Toys were recorded with a Spectrasonics mixing board and a 16-track tape recorder. By this point, Aerosmith had fully matured as a band and Steven Tyler made sex the primary focus of his songwriting on the album.
According to producer Jack Douglas, "Aerosmith was a different band when we started the third album. They'd been playing Get Your Wings on the road for a year and had become better players - different. It showed in the riffs that Joe and Brad brought back from the road for the next album. Toys in the Attic was a much more sophisticated record than the other stuff they'd done." In the band memoir Walk This Way, guitarist Joe Perry concurs, "When we started to make Toys in the Attic, our confidence was built up from constant touring." In his autobiography, Perry elaborates:
Aerosmith's third album includes some of their best known songs, including "Walk This Way", "Sweet Emotion", and the rollicking title track. "Walk This Way" starts out with a two measure drum beat intro by Joey Kramer, followed by the well known guitar riff by Joe Perry. The song proceeds with the main riff made famous by Perry and Brad Whitford on guitar with Tom Hamilton on a Rickenbacker bass. The song continues with rapid fire lyrics by Steven Tyler. The song originated in December 1974 during a sound check when Aerosmith was opening for The Guess Who in Honolulu. During the sound check, Perry was "fooling around with riffs and thinking about The Meters", a group guitarist Jeff Beck had turned him on to. Loving "their riffy New Orleans funk, especially 'Cissy Strut' and 'People Say'", he asked the drummer "to lay down something flat with a groove on the drums." The guitar riff to what would become "Walk This Way" just "came off hands." Needing a bridge, he:
played another riff and went there. But I didn't want the song to have a typical, boring 1, 4, 5 chord progression. After playing the first riff in the key of C, I shifted to E before returning to C for the verse and chorus. By the end of the sound check, I had the basics of a song.