Dimitrov, 23, played superbly to win 6-1 7-6 (7-4) 6-2 in two hours and one minute and reach his first Grand Slam semi-final.
Murray had been on a 17-match winning streak at Wimbledon and was looking to reach his sixth
consecutive semi-final.
It is the first time since 2008 that he has failed to make the last four.
Dimitrov, seeded 11th, had too much with his big serve, variety of shots and athletic defence for an off-key Murray, who looked underpowered on serve and made a host of unforced errors.
The atmosphere on Centre Court was in marked contrast to 12 months ago, when 15,000 thrilled spectators watched Murray become the first Briton since Fred Perry in 1936 to win the men's singles.
In the year that followed, Murray had undergone back surgery in September and lost the services
of coach Ivan Lendl in March, with Frenchwoman Amelie Mauresmo stepping into the role on the
eve of Wimbledon.
But only four men in the open era - Bjorn Borg, Boris Becker, Pete Sampras and Roger Federer - had returned after their first Wimbledon victory to defend the title, and despite impressing in the earlier rounds, Murray fell well short against Dimitrov.
"My start to the match was poor," said Murray.
"I started the match badly and I think that gave him confidence.
"I should have done a better job at the beginning of the match of making it tougher for him, and I didn't manage to do that.
"Also, when I got back into the second set, that was my opportunity there."
The 27-year-old Scot, whose run at SW19 included his 2012 Olympic gold and last year's Wimbledon triumph, could not convert a break
point in a tight opening game, and Dimitrov grew in confidence from the opening four-minute test.
He had little trouble returning the Murray serve and, unlike the Briton's previous opponents, was able to dictate in the longer exchanges.
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