The British rock band was among the star-studded line-up at the world famous festival, held at the Empire Polo Club in Indio, California, over the weekend.
During their Saturday slot, the group performed a host of their hits including Song 2, Beetlebum and Tender.
As the band struck up the chords to their 1994 hit Girls & Boys, lead singer Albarn tried encourage the crowd to sing along to the chorus saying: "I need your participation, please."
In videos shared to social media, he can be seen attempting to engage the concert-goers a number of times, telling them "You can do it better than that", but his efforts continued to receive a lacklustre response from the US crowd.
The musician appeared to get increasingly frustrated until he told the audience: "You'll never see us again so you may as well f***ing sing it."
Dressed in a white suit and a black T-shirt paired with a pair of black sunglasses, frontman Albarn led the band which also consists of guitarist Graham Coxon, bass guitarist Alex James and drummer Dave Rowntree.
Formed in 1988, the English band have released nine albums across their career including 1994's Parklife, 1995's The Great Escape, 1997's Blur, 1999's 13, 2003's Think Tank and 2015's The Magic Whip - which all went to number one in the charts.
The group helped pioneer the Britpop genre, fiercely competing with rival band Oasis in the charts over the years.
They went on a hiatus after their 2015 Magic Whip tour, but came back last year with their first record for eight years, titled The Ballad Of Darren, which soared to number one.
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