The concept to which The Rascals were dedicated was, in Felix Cavaliere's words, "Marvin Gaye's voice, Ray Charles' piano, Jimmy Smith's organ, Phil Spector's production and The Beatles' writing. Put them all together and you've got what I wanted to do." A White Rock band playing Black Soul music was a new idea for Pop in 1965. "The great thing about music in the 1960s was that people were discovering there was no color barrier in the business. We were respected by the Black groups we loved as much as we respected them," noted Cornish. The Rascals' music was dubbed blue-eyed Soul, a term Cavaliere never cared for. "I always hated the label because it created a separation between Black and White music. It was a marketing concept. As soon as you put a drum in music, it's R&B. I wish it wouldn't have been called blue-eyed Soul. My eyes aren't blue."

The band's first release for Atlantic was called "I Ain't Gonna Eat Out My Heart Anymore" which rose to #52 in the U.S. in 1965, but it was their 1966 effort, "Good Lovin'" that made them Rock 'n' Roll stars. The song quickly rose to the number one spot on Billboard's Hot 100 and went Gold. They followed with two more Top 20 hits, "You Better Run" (#20) and "I've Been Lonely Too Long" (#16) later the same year.

The writing was a key component of the band's success, as sixteen of their eighteen chart records were written by Cavaliere alone or in tandem with frequent collaborator Eddie Brigati. As the song writing progressed, social commentary began to show up in the music. The group's growing ambition was reflected in the change from The Young Rascals to simply The Rascals. The word "young" had originally been inserted before the band's name for legal reasons. It seems there was a group named Johnny Pulleo & The Harmonica Rascals who claimed a proprietary interest. "We were embarrassed about that, 'cause we were trying to be a Soul band," said Cornish. "It wasn't The Silver Rascals or The Rockin' Rascals, it was The Young Rascals! And we had to live with it. By the time we got to Groovin', we said, 'Well, enough of this. We are The Rascals.'"

A high point for both Cornish and Cavaliere was 1968's #1 hit "People Got To Be Free". "The message in songs like 'People Got To Be Free' is as important now as it ever was," said Gene. It was written in reaction to the King and Kennedy assassinations that year. In fact, Cavaliere had worked for the RFK campaign. "That the song was #1 in places like Berlin and South Africa meant a lot to me," said Felix. Despite the initial resistance to the political nature of the song, it went on to become The Rascals' biggest-selling record. It was also their last #1 hit. The Rascals followed with "A Ray Of Hope" (#24 in 1968), "Heaven" (#39 in 1969), "See" (#27 in 1969) and "Carry Me Back" (#26 in 1969). Two other 1970 releases, "Hold On" (#81) and "Glory Glory" (#71) failed to crack the Top 40, and a song called "Love Me" was a miserable flop when it peaked at #99 during a one week stay on the Hot 100 in the Summer of 1971. The Jazz-tinged experimentation of later albums like "Peaceful World" and "The Island Of Real" (which Cavaliere once called "The best record I ever made") proved less commercial than the group's earlier Garage Band Soul. Management was less than supportive of the new directions the band was headed in and a switch to the Columbia label in 1971 failed to provide the new life they were looking for. Personal frictions were on the rise too, and eventually Brigati and Cornish quit the band. They were replaced with Buzzy Feiten (from The Paul Butterfield Blues Band) and Ann Sutton, who had sung with various Soul and Jazz groups in Philadelphia. By 1972, The Rascals called it quits.