In 2006, Hot Chip released their second album, The Warning. Now signed to EMI in the UK, the band gained more mainstream appeal as well as the attention of critics. The album was shortlisted for the 2006 Nationwide Mercury Prize and was Mixmag's Album of the Year 2006. This album spawned also two UK top forty singles: "Over and Over" in March 2006 and "Boy from School" in May 2006. "Over and Over" received attention for its music video, which was directed by Nima Nourizadeh, and was also named as the best single of 2006 by British music magazine NME.

The band released their third studio album, Made in the Dark, on February 4, 2008. The first song to be released from it was "Shake a Fist", which was released as a limited one-sided 12" in August 2007. The second release was "Ready For The Floor" in January 2008, which reached number 6 on the UK Singles Chart in the United Kingdom. In order to promote "Ready for the Floor", the band appeared on Friday Night with Jonathan Ross in January 2008, and Joe Goddard appeared on Never Mind The Buzzcocks on 31 January. In February 2008, the band performed on the American talk shows Jimmy Kimmel and Carson Daly. At the end of 2008, "Ready For The Floor" received a Grammy Award for Best Dance Recording nomination, but the song later lost out to "Harder, Better, Faster, Stronger" by Daft Punk. On 7 May 2008, the group performed their third single, "One Pure Thought", on Radio 1's Live Lounge. The hypnotic clip for "One Pure Thought" was selected as one of the best music videos of 2008 by AllMusic.com.

Having completed a world tour in February 2009, Hot Chip returned to London and began writing and recording their fourth album, One Life Stand.

In early 2009, Alexis Taylor told NME that the band recorded new songs including "Alley Cats", which the band played regularly while touring in 2008/2009. Initially, Taylor hinted that the album was going to be "a bit calmer this time" in comparison to Made in the Dark with songs that are "more mid-tempo and disco influenced", although the two tracks released prior to the album, "Take It In" and "One Life Stand", suggest that it will be more upbeat than first suggested, and may be more influenced by early house music. Alongside the regular band members, Hot Chip collaborated on several of the album tracks with the drummer Charles Hayward from This Heat and Camberwell Now, Leo Taylor, drummer from the London based band The Invisible and the Trinidadian steel pan player Fimber Bravo.

One Life Stand was released on 1 February 2010.

Their self-produced fifth studio album In Our Heads was released on 11 June 2012 by Domino.

About the album, Alexis Taylor stated, "I think “In Our Heads” was a bit speedier, and made with less pressure, but more fun – partly due to people in the band not having too many hang ups about how good the material was – we seemed to be happy with the songs we were writing and they came quickly – and partly due to the fact that we had been enjoying ourselves elsewhere, whether at home, or on tour, or recording with our other projects, or DJing. I think that is right about subtler confidence, but it may also be that we are a bit more accepted these days as we keep doing what we want, and gradually people stop saying ‘why’ to everything and each decision. The songwriting developed quickly from songs that were dreamt ("Now There is Nothing"); songs that were written via email file sending (fully fleshed out instrumentals from Joe developing into songs with added percussion/chord changes and singing by me; e.g. "Flutes"); songs that we bashed out in collaborative writing sessions between Joe and myself ("Don’t Deny Your Heart", "How Do You Do?"); songs that one or the other of us wrote largely separately "‘These Chains’"– Joe/"Look At Where We Are"- Alexis); songs that a few of us in the room wrote more of: "Dark and Stormy", or to some extent "Let Me Be Him" (at least in chorus terms); or finally songs that were written after we completed the last album and which were still in our minds: "Always Been Your Love", "Doctor"."

During live performances, Hot Chip reinvent their studio compositions to form what has been described by Glide magazine as "heavy beat-driven improvisation" that create "an atmosphere of excitement, energy and the unexpected." Festival appearances include V Festival 2008, Dour Festival, Glastonbury, Treasure Island Festival, Roskilde festival, Sónar, Benicassim, Electric Picnic, Bestival, Lovebox, Bonnaroo, the Reading and Leeds Festivals, the Big Day Out, Melt! festival, T in the Park, Summer Sundae, Splendour In The Grass, Lollapalooza in 2006 and 2010, the Brazilian Tim Festival in 2007, Oxegen in 2008, Coachella in 2007, 2008, 2010 and 2013, Way Out West Festival in 2012, Austin City Limits in September 2008, and Ultra Music Festival in 2013.

During a performance at the Glastonbury festival on 28 June 2008, Hot Chip played their cover of "Wearing My Rolex" and were joined onstage by Wiley. They also ended a number of sets in 2008 with a cover of Prince's (popularised by Sinéad O'Connor) "Nothing Compares 2 U." Returning to the festival in 2010 they performed a version of their song "I Feel Better" with a steel pan ensemble known as "Steel Harmony".

In the latter half of 2010, having toured extensively in the USA, Japan, Australia and Europe, the band united with long term collaborators and friends LCD Soundsystem to play shows in the US and the UK, including a joint headline show at Alexandra Palace in London. In Salt Lake City, UT, on a one-off headlining show on 19 October 2010, they debuted a new song, "Ends of the Earth," for an upcoming album. Al Doyle said at the concert that the new album could be released in 2011.

This was followed by a series of shows in South America and Mexico, including debuts in Chile and Colombia. Their final show of the "One Life Stand" tour was at the YOTA Festival of Light in the Russian city of St Petersburg on December 4, 2010.

The band is also known for its DJ talent; they have released several mix CDs and mixes for national and international radio stations and they all DJ regularly worldwide.

Hot Chip released a DJ-Kicks compilation album in 2007, which included a new song called "My Piano", also released as a 12".

In 2008, the band released an EP which included collaborations with Robert Wyatt. Wyatt sang and reworked versions of three tracks from Made in the Dark, and the Hot Chip with Robert Wyatt and Geese EP also included a remix by Geese, a string quartet based in London who have regularly contributed to Hot Chip's recordings. Alexis Taylor also released a solo album in late 2008 entitled Rubbed Out, which saw him focusing more on the fundamental sounds used by Hot Chip leading to a more downtempo and bluesy album than Taylor's works with Hot Chip.

In 2009, a new DJ mix album A Bugged Out Mix by Hot Chip was released on the Bugged Out label, a two disc album with disc one a collection of club and dance tracks mixed by Martin, and disc two a "house party" mix put together by Goddard, Taylor and Clarke. The artwork was made by Bevis Martin and Charlie Youle.

Other releases in 2008-2010 included a collaboration with Peter Gabriel on a cover version of the Vampire Weekend song Cape Cod Kwassa Kwassa, many remixes including the song "Babongo Tribe Remix" for the Survival International charity album, Songs for Survival and a cover of Joy Division's "Transmission" to the War Child charity album, Heroes. A collaboration between Alexis Taylor, Joe Goddard and Bernard Sumner entitled "Didn't Know What Love Was" was released in October 2010.