He staged the premiere of "folk opera" Dr Dee, about the ill-fated scientist and occultist John Dee, in Manchester.
The show sees the Blur singer peform songs on a platform above the stage while actors and opera singers take part in an elaborate production below.
It will move to the home of the English National Opera in London next summer.
Bertie Carvel (front) plays John Dee Albarn, who also fronts the pop band Gorillaz, has said Dr Dee has been the most difficult challenge and the most important project of his career.
The show, directed by Rufus Norris, was inspired by Albarn's fascination with Dee and his lasting influence on English identity.
Dee was a scientific and medical adviser to Elizabeth I who advocated the creation of a British Empire, helped explorers navigate the New World and held seances in the hope of finding a key to unlock the secrets of nature.
William Shakespeare is believed to have based the sorcerer Prospero, from The Tempest, on Dee.
The production started by tracing modern English identity back to Dee's era, before charting his life story, from mathematical brilliance in the Elizabethan court to dark and brooding scenes of downfall.
Throughout the performance, Albarn was perched on a platform above the stage, wearing a black leather jacket and jeans rather than the baggy breeches and ruffs sported by the actors.
He picked up his acoustic guitar and broke into song at regular intervals, acting as a modern-day musical commentator on the action below and drawing parallels between the Englands of the 16th and 21st Centuries.
He was joined on the platform by a small band that included the Nigerian drum legend Tony Allen and musicians playing period instruments such as the rackett, the viol, the crumhorn and a large lute called the theorbo.
Watch Albarn perform a song from the opera on The Andrew Marr ShowAlbarn was initially reluctant to describe the production as an opera, but has since summed it up by defining it as an English folk opera.
"It's an ongoing dilemma - what do you call something that's new?" he recently told BBC Radio 4's Front Row.
There was praise among the audience for the staging, with its continually inventive use of props, projections and powerful symbolism.
Dr Dee is one of the showpiece productions at the third Manchester International Festival.
The festival takes place every two years and Albarn has been involved at every event so far.
His first foray into opera, with the spectacular Chinese performance piece Monkey, was among the highlights of the first festival in 2007.
John Dee died in poverty and isolation after a posting to Manchester in 1596 But Albarn did not perform in that show. He said he needed to appear in Dr Dee because it was "a chance to express something about England".
"I've got a really strange emotional connection, and it really gets to me - that haunted, magical England," he told Front Row.
"It's something that really stirs me in an irrational way. The only way I could honestly write about Dee was to involve myself in the whole thing. But I'm not walking around in a ruff and tights."
John Dee spent the latter part of his life as warden of Manchester College and Albarn has had access to Dee's letters at the city's John Rylands Library.
"Manchester has become creatively like a second home for me in this country," the singer said.
Dr Dee can be seen at the Palace Theatre in Manchester until 9 July and will open at the London Coliseum as part of the London 2012 Festival for the Cultural Olympiad next June.
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