The first of his singles that got airplay outside of New Orleans was "Over You." Neville's first major hit single was "Tell It Like It Is," which topped Billboard's R&B chart for five weeks in 1967 and also reached No. 2 on the Hot 100. It sold over one million copies, and was awarded a gold disc. A remake of the song was a top 10 pop hit for the rock group Heart featuring Ann and Nancy Wilson in 1981.

In 1989, Neville teamed up with Linda Ronstadt on the album Cry Like a Rainstorm, Howl Like the Wind. Among the duets recorded for the disc were the #1 Grammy-winning hits "Don't Know Much" and "All My Life". "Don't Know Much" earned a million-selling Gold single, while the album was certified Triple Platinum for US sales of more than 3 million.

His other hits have included "Everybody Plays the Fool," his 1991 cover of the 1972 Main Ingredient song, that reached No. 8 on the Hot 100; "Don't Take Away My Heaven," "Hercules" and "Can't Stop My Heart From Loving You (The Rain Song)." Neville's biggest solo successes have been on the Adult Contemporary chart, where "Don't Know Much," "All My Life" and "Everybody Plays the Fool" all reached No. 1 in 8 European countries.

In August 2005, his home in Eastern New Orleans was destroyed by Hurricane Katrina. He evacuated to Memphis, Tennessee, before the hurricane hit. He moved to Nashville after the storm, and had yet to return to the city as of early 2008, causing the New Orleans Jazz and Heritage Festival to temporarily change its tradition of having the Neville Brothers close the festival. However, the Neville Brothers, including Aaron, returned for the 2008 Jazzfest, which returned to its traditional seven-day format for the first time since Katrina. Neville is in the process of moving back to the New Orleans area, namely the North Shore city of Covington. Neville performed Randy Newman's "Louisiana 1927" during NBC's A Concert for Hurricane Relief on September 2, 2005.

Neville signed to SonyBMG's new Burgundy Records label in late 2005 and recorded an album of songs by Otis Redding, Marvin Gaye, Curtis Mayfield, Sam Cooke and others for Bring It on Home... The Soul Classics, released on September 19, 2006. The album, produced by Stewart Levine, features collaborations between Neville and Chaka Khan, Mavis Staples, Chris Botti, David Sanborn, Art Neville, and others. The album's first single was a remake of The Impressions' 1963 classic "It's All Right."

Neville's career has included work for television, movies and sporting events. Neville sang the National Anthem in the movie "The Fan," starring Robert De Niro and Wesley Snipes. In 2006, Neville performed "The Star-Spangled Banner", alongside Aretha Franklin and Dr. John on keyboards at Super Bowl XL in Detroit, Michigan. In addition, Neville did background vocals for the songs "Great Heart," "Bring Back the Magic," "Homemade Music," "My Barracuda" and "Smart Woman (in a Real Short Skirt)" on Jimmy Buffett's Hot Water, released in 1988.

In 2008 he released Gold, which includes a double album of his hits.

On December 12, 2010, while performing at Baton Rouge's Manship Theater in the Shaw Center, Neville was inducted into The Louisiana Music Hall Of Fame. Neville is also an inductee of the Delta Music Museum Hall of Fame in Ferriday, Louisiana.

In 2013, paying tribute to the songs of his youth, Blue Note Records released Neville's My True Story, a collection of 12 doo-wop tunes, produced by Don Was and Keith Richards, with backing by musicians such as Benmont Trench and Tom Petty and the Heartbreakers.

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