Nathan Williams started his professional music career at 21, just five years after high school, recording singles for his brother's El Sid label. Sid also opened a venue in Lafayette, El-Sid-O's, where Nathan became a staple performer on Friday nights. 

During a period of illness recovery, Williams chose to devote himself to mastering the accordion, practicing secretly in the bathroom. He looked up to Buckwheat Zydeco, who was a key mentor, but it was Chenier who left a lasting impact on his music. Sid eventually bought Nathan his first accordion from Buckwheat Zydeco.

His big break came when he was recommended to Rounder Records by Buckwheat Zydeco as his accordionist replacement after Buckwheat left for Island Records. 

In 1985, inspired by a Chenier instrumental, he founded Nathan & the Zydeco Cha-Chas. The band debuted at the New Orleans Jazz & Heritage Festival in 1988. In November 1992, the Cha Chas played at the New Orleans Rock n' Bowl for the first time, paving the way for regular zydeco nights there starting in spring 1993. Nathan's 1997 live album, "I'm a Zydeco Hog: Live at the Rock 'N' Bowl, New Orleans," captured the energy of these performances. They also celebrated the venue's 30th anniversary in 2018.

The New York Times once noted that Williams, at 25, was "poised to become important" in revitalizing zydeco. His music blends zydeco, jazz, blues, and R&B, with most of the band’s original songs penned by Williams.

For over three decades, Nathan & the Zydeco Cha Chas have toured extensively, performing everywhere from local Louisiana spots to international stages in countries like Austria, Spain, France, Japan, the Netherlands, Turkey, Germany, and even Poland, a first for a zydeco band.

Led by Nathan Williams as songwriter, founder, vocalist, and accordionist, the Cha Chas include his brother Dennis Paul on guitar, cousin Alan Williams on bass, Jaston George on rubboard, and Keith Sonnier on drums. Nathan’s uplifting, roots-inspired music is served up with a distinctive Caribbean lilt that reaches back to the very beginnings of Louisiana Creole culture.