Two years later, Aaron scored his first solo hit, "Over You"; in 1966, he notched a pop smash with the classic "Tell It Like It Is," a lush ballad showcasing his gossamer vocals. Art, meanwhile, returned from the service to begin his own solo career, and recorded a series of regional hits like "Cha Dooky Doo," "Zing Zing" and "Oo-Whee Baby." In 1967, he formed Art Neville and the Sounds, which included both Aaron and Charles as featured vocalists and quickly became a sensation on the local club circuit.

In 1968 producer Allen Toussaint hired the group as the house band for his Sansu Enterprises; minus Aaron and Charles, the Sounds evolved into a highly-regarded rhythm section which backed artists as diverse as Lee Dorsey, Robert Palmer and Labelle before eventually finding fame on their own as the Meters. Consequently, Aaron resumed his solo career, although with only sporadic success; as a result, he also worked as a dock hand. Charles, meanwhile, relocated to New York City, where his skills as a saxophonist led to tenures with a variety of jazz units; after returning to New Orleans, he was arrested for possession of marijuana and served a three-year sentence at the Angola Prison Farm.

In 1975, the Meters backed the Wild Tchoupitoulas, a group led by the Nevilles' uncle, George "Big Chief Jolly" Landry. Both Aaron and Charles were enlisted for the session, as was youngest brother Cyril; when the Meters disbanded the following year, the four brothers backed the Tchoupitoulas on tour, and in 1977 they offically banded together as the Neville Brothers. Despite their gift for intricate four-part harmonies, their self-titled 1978 debut unsuccessfully cast the vocal quartet as a disco band, and following a dismal response they were dropped by their label, Capitol.

The Nevilles spent the following three years without a contract, but after signing with A&M, fan Bette Midler helped secure the services of producer Joel Dorn for 1981's superior Fiyo on the Bayou, which spotlighted Aaron's angelic tenor on standards like "Mona Lisa" and "The Ten Commandments of Love" along with renditions of "Iko Iko" and "Brother John." Despite widespread critical acclaim, the album sold poorly, and again the Nevilles were cut loose from their contract. After signing to the tiny Black Top label, they issued 1984's Neville-ization, an incendiary live set recorded at the Crescent City landmark Tipitina's which featured Duke Ellington's "Caravan" and Aaron's perennial "Tell It Like It Is" alongside the brothers' own "Africa" and "Fear, Hate, Envy, Jealousy."

After another concert album, 1987's Live at Tipitina's, the Nevilles signed with EMI and returned to the studio in 1987 with Uptown, which again met with commercial failure despite cameo appearances from Keith Richards, Jerry Garcia and Carlos Santana. In 1989, they re-signed to A&M and recruited the services of famed New Orleans producer Daniel Lanois; the atmospheric Yellow Moon, the group's finest hour, finally earned them success on the charts, thanks in part to the anthemic single "Sister Rosa." 1990's Brother's Keeper fared even better, no doubt spurred by Aaron's concurrent success with Linda Ronstadt on the smash duet "Don't Know Much."

In addition, a second generation of Nevilles also began making their mark on music; in 1988, Aaron's son Ivan, a member of Keith Richards' backing band the X-Pensive Winos, released his solo debut, If My Ancestors Could See Me Now. The Neville Brothers legacy continued in 1999 with Valence Street.