On 28 January 2006, with other surviving members of the Bonzo Dog Doo-Dah Band, Smith played a reunion concert at the London Astoria. A countrywide tour, which began in Ipswich and ended with two shows at the Shepherd's Bush Empire, with Ade Edmondson and Phill Jupitus, followed during November 2006. The Shepherd's Bush Empire shows were filmed for TV broadcast by the BBC and also released on DVD. A further sold-out concert at the London Astoria in June 2008 saw Smith perform with the Bonzo Dog Doo-Dah Band where his 'Mr Wonderful' stage persona was a highlight of the concert.
In March 2009, Smug Records released Legs" Larry Smith's – 'Call Me, Adolf!', a five-track digital EP produced by Gus Dudgeon.