The duo met when Sitek moved into the building where Adebimpe had a loft; each of them had been recording music on his own, but realized their sounds would work well together. Sitek's brother Jason began playing drums and other instruments with the pair during their recording sessions, which resulted in a self-titled, 24-track CD released by the Brooklyn Milk imprint. Jason Sitek left the band for a short time due to other musical commitments but returned to the band when they recorded their Touch and Go debut, the Young Liars EP.
After the EP was completed, TV on the Radio added guitarist/vocalist Kyp Malone to their fold. Young Liars, which also features the Yeah Yeah Yeahs' Brian Chase and Nick Zinner, was released in summer 2003 to critical acclaim, coinciding with their gigs opening for the Fall. Their first full-length release, Desperate Youth, Blood Thirsty Babes arrived in spring 2004. The band remained busy for the rest of the year, embarking on their own tours as well as dates with the Faint and the Pixies. That fall, they released the New Health Rock EP and won the 2004 Shortlist Prize.
In 2005, the band kept busy with touring and returned to Sitek's Stay Gold studio to work on their second album. They also made an MP3 criticizing President George W. Bush, "Dry Drunk Emperor," available on their website. TV on the Radio signed with 4AD for European distribution of their albums and moved to Interscope in the U.S. In summer 2006 they resurfaced with Return to Cookie Mountain, a more polished but still searching collection of songs that featured David Bowie on backing vocals. The band went in a sleeker direction on 2008's Dear Science, which featured cameos from Antibalas and Celebration's Katrina Ford.