Hound hosted the year 2000 edition of My Funniest Year, a look at a past year of British television, which was broadcast on Channel 4 in September 2010. He has been a regular panelist on Celebrity Juice, hosted by Keith Lemon, and has appeared at Bright Club a number of times. In January 2011, Hound participated in the former Channel 4 reality series Famous and Fearless. He came third for the boys' team, and was referred to as "The Ruthless Hound". In 2012, Hound was a team captain for Mad Mad World.

Hound hosted Destination Three, the coverage of the Glastonbury Festival and Top of the Pops in 2005 and 2006 alongside Fearne Cotton. He presented the idiosyncratic reality show Grime Scene Investigation on BBC Three with staff and students from Aston University, and narrated BBC Two's broadcasts of MythBusters. He has also appeared in many comedy shows and quizzes such as Street Cred Sudoku, Nevermind the Buzzcocks and Celebrity Juice, where he was a regular panellist. He narrated the 2009 series Rocket Science and has appeared on The Apprentice: You're Fired! and Richard & Judy. He also presented Outtake TV on BBC1, replacing Anne Robinson.

In April 2007, Hound was married at the Little White Wedding Chapel in Las Vegas, Nevada to Beth Johnson, whom he had met at the Reading Festival the year before. They have two children together.

In early 2008, Hound appeared twice on ITV's Thank God You're Here in the UK, after initially working as the warm-up act. In late summer 2008, Hound joined the panel show Argumental as the Blue Team Captain. Hound was the narrator for the Gaming series Playr and presents What Do Kids Know? on UKTV-owned channel Watch. Hound took part in Let's Dance for Sport Relief, dancing to Cheryl Cole's "Fight for This Love" and won the final of the series on 13 March 2010. Partnered with Flavia Cacace, Hound won the 2013 Strictly Come Dancing Christmas special.

Hound made his acting debut in the Direct-to-DVD film Big Fat Gypsy Gangster which was directed by Ricky Grover. He also stars in the 2012 film The Wedding Video.

From October 2012 through February 2013, Hound played the lead role of Francis Henshall in the National Theatre's second touring production of One Man, Two Guvnors. Following the end of the tour, he took over the role in the West End production from 4 February 2013.

Hound campaigned for the Liberal Democrats at the 2010 general election. He has subsequently declared his support for the Labour Party. In an episode of The Jonathan Ross Show, which aired on 25 January 2014, Hound announced plans to run as a Member of the European Parliament for the party in the London constituency. Hound was the fifth candidate on the National Health Action Party list, which came ninth, receiving 23,253 votes (1.06 per cent of the vote).

In August 2015, Hound endorsed Jeremy Corbyn's campaign in the Labour Party leadership election. He tweeted: "Understand your thinking, but Corbyn=alternative. The others =Tory policies inflicted with mea culpa eyes". In July 2016, he also supported Corbyn after mass resignations from his cabinet and a leadership challenge. He performed stand-up at "Keep Corbyn event" in Kentish Town and tweeted: "About to go on. #istillbelieve #jc4pm".

In late 2016, he played Toad in the world premiere of the new musical, The Wind In The Willows in Plymouth, Salford and Southampton. In June 2017 he will reprise the role for a West End transfer at the London Palladium, after playing Dr Prentice in What The Butler Saw by Joe Orton at the Curve Theatre, Leicester and Theatre Royal Bath in March 2017.

In May 2017, Hound wrote a series of Tweets concerning the 2017 Manchester Arena bombing in which he implied the attack was a false flag attack, designed to help the Conservative Party in the upcoming general election, likening it to the German Reichstag fire of 1933.