The 32-year-old Swiss slumped to a 6-7 (5/7), 7-6 (7/3), 6-2, 4-6, 6-3 fourth round loss to 18th seeded Ernests Gulbis -- his earliest Paris exit since 2004 when he was demolished in the third round by Gustavo Kuerten.
It was Federer's first five-set loss in his French Open career and thwarted his hopes of playing in a record 42nd Grand Slam quarter-final and 10th in a row at Roland Garros.
But in the immediate aftermath of his defeat, Federer insisted that rather than carrying out a post-mortem on his Paris campaign he was already setting his sights on Wimbledon and clinching a record eighth title.
"Yeah, I do feel so," said Federer when asked if another title at the All England Club was still within his grasp.
"I think when I'm healthy, like I have been now for the last six to nine months, I think clearly I can also decide the outcome of the matches more than I could last year," he said.
"So I'm very excited about my chances for Wimbledon now this time."
Federer won his seventh Wimbledon title in 2012, equalling the mark of Pete Sampras.
It was his 17th career major but also his most recent.
Last year, his challenge was ended in the second round by Ukraine journeyman Sergei Stakhovsky and should he triumph in London later this month he would succeed Arthur Ashe as the oldest men's champion.
The American was 31 when he lifted the title in 1977; Federer will be 33 in August.
Federer's only French Open triumph came in 2009 and his last three visits to Paris have yielded steadily diminishing returns.
After finishing runner-up in 2011 to Rafael Nadal, he was a semi-finalist in 2012, a quarter-finalist in 2013 before his last-16 exit to outspoken Latvian player Gulbis on Sunday.
"Mentally I have already switched to the grass, to be quite honest," Federer said.
"For me, it's like, okay, clay court season was fun, but we are moving on," he said.
"Clay doesn't need me anymore, I got flushed out here."
But Federer had his chances on Sunday.
After wrapping up the first set, he had two set points in the ninth game of the second before he was broken by the big-hitting Gulbis who unleashed 13 aces and 53 winners in a Philippe Chatrier court contest where the Swiss was the overwhelming favourite with the Paris crowd.
But Federer wasn't helped by an uncharacteristic 59 unforced errors as Gulbis varied the pace and the angles, forcing the Swiss to hit more and more forehands to reduce the threat.
"I guess I was a bit all over the place," Federer said.
"Clearly very disappointed not to come through with the win," he said.
"After the chance in the second set, fighting back in the fourth, not to play a better fifth set."
Federer acknowledged he had a lot of regrets.
"But I think Gulbis did a good job of hanging around and clearly coming back in that second set was crucial for him, I think," he said.
"So it was a tough match and I'm disappointed I lost it."