The US rockers performed a set of their biggest hits - including 'Numb', 'Faint', 'Crawling' and 'One Step Closer' - before surprising fans with their version of the soul singer's huge hit during their encore at Camden's Roundhouse in London.
Before they performed the track lead vocalist Chester Bennington teased the audience, saying: "We're going to do something really special for you guys, this is something we don't usually do. We're going to play a song by a local artist."
The band's version of Adele's UK and US number one single saw the band stripped back, with Chester singing and multi instrumentalist Mike Shinoda playing the piano.
The hit was part of a five-song encore that saw the band - who are also made up of drummer Rob Bourdon, lead guitarist Brad Delson, bassist Dave Farrell and DJ Joe Hahn - close the night with energetic performances of their 2001 single 'In The End' and 2007's 'Bleed It Out'.
Chester told the crowd: "It feels good to be down here with a bunch of people who really want to f***ing be here."
They band opened with 'The Requiem' before launching into 'Papercut' and also performed 'No More Sorrow' and 'Breaking the Habit' during their set.
Linkin Park's set at the iTunes festival 04.07.11:
Lying From You
What I've Done
When They Come for Me
No More Sorrow
Jornada del Muerto
Waiting for the End
Burning in the Skies
Breaking the Habit
One Step Closer
Rolling in the Deep (Adele cover)
Wisdom, Justice, and Love
In the End
Bleed It Out