The Swiss fourth seed, who won the title in 2009, seemed to have the match in his grasp against the unpredictable Gulbis but faded badly to lose 6-7(5) 7-6(3) 6-2 4-6 6-3.
It is the first time since 2004 that 32-year-old father of four Federer has failed to reach the quarter-finals and he has now fallen before that stage in three of his last four grand slams tournaments.
Seventh seed Murray reached the fourth round, winning a deciding set 12-10 against Germany's Philipp Kohlschreiber having re-started the match on Sunday locked at 7-7 in the fifth after bad light stopped play the previous evening.
In the women's singles fast-rising Canadian Eugenie Bouchard thrashed Angelique Kerber 6-1 6-2 to claim a quarter-final spot, crunching 30 winners in 52 dazzling minutes to stretch her winning run on clay to nine matches.
Former world No.1 Federer, who became father to a second set of twins recently, looked a slightly forlorn figure as Gulbis turned around the match and the days when he was a near certainty to reach semi-finals appear to be over.
The 17-times grand slam champion was beaten in the second round at Wimbledon last year and the last 16 at the U.S. Open although he did enjoy a semi-final run in Australia.
On yet another gloomy day in Paris after some welcome sunshine on Saturday, Federer never looked comfortable against Gulbis, who said earlier this week he was hoping to catch the "last-chance train" after under-achieving since reaching the quarter-finals of the Frecnh Open in 2008.
"It is the biggest win of my career. I had to win, I know how all of you love Roger but that's sport," world No.17 Gulbis said on the court as the stunned fans looked on.
"I won tournaments in Marseille and Nice so hopefully Paris is the next one. I win, I win over some fans," he added, looking ahead to his next match against sixth seeded Czech Tomas Berdych who ended U.S. interest in the men's singles with a 6-4 6-4 6-4 trouncing of towering John Isner.
Federer, who squandered two set points for a two-set lead, left court Philippe Chatrier head bowed after allowing Gulbis to come back and dominate with some relentless attacking tennis.
GUNS BLAZING
At 5-2 in the fourth set Gulbis took a medical timeout and he came back with all guns blazing to break Federer's serve immediately, on the way to winning 10 of the next 11 points against a visibly rattled opponent.
Federer still managed to take the set but he was never the same again and Gulbis controlled his own suspect temperament to claim victory when a Federer backhand went wide.
Murray, who had been cramping the previous evening after failing to finish off Kohnschreiber, had to play inspired tennis to finally finish off the German who succumbed when asked to serve to stay alive for the seventh time in a gripping finale.
"When you start 7-7 every single point counts," Murray, who had not played a five-setter since returning from back surgery, told reporters. "Today was a pretty high standard, probably the best standard of the match I think from both of us."
He will play Spain's Fernando Verdasco next after he also returned to finish off Frenchman Richard Gasquet with ease.
With so many top seeds gone from the women's draw 20-year-old Bouchard is now looking like a serious title contender.
The 18th seed, who reached the Australian Open semi-final this year, completely outclassed Kerber and after her first WTA title last week in Nuremberg she is flying high.
"I feel like since the beginning of the year I have been improving my game, since Australia I'm at a different level from there," Bouchard said.
"I have confidence in myself. I can play like this and play even better," she added.
Her pace and variety of shots were too much to handle for the higher-seeded Kerber, who had reached the last eight at Roland Garros in 2012.
The German was caught snoozing early on and went 5-0 down, never recovering as Bouchard set up a meeting with 14th seed Carla Suarez Navarro after the Spaniard used her one-handed backhand to great effect to end the run of up-and-coming Croatian Ajla Tomljanovic with a 6-3 6-3 win.
It proved a good day for Canada with eighth seed Milos Raonic reaching the quarter-finals after an emphatic 6-3 6-3 6-3 victory over Spain's Marcel Granollers.
He will face world number two Novak Djokovic in the last eight if the Serb beat Frenchman Jo-Wilfried Tsonga later.
(Reporting by Julien Pretot; Editing by Martyn Herman)
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