Mahut, the 2008 finalist and now the world number 65, raced through the third-set tiebreak, taking the first six points to win 7-1.
He needed only two of the six match points, with Murray slicing a backhand into the net to end proceedings.
The Frenchman will now play Bulgarian Grigor Dimitrov while Murray, the world number four who was beaten in the French Open quarter-finals, must find another way to prepare for the start of Wimbledon on June 25.
"Maybe it's the best victory of my career, it was a difficult match and I'm very happy," Mahut, who will always be remembered for a record 11 hour five minute tussle with American John Isner at Wimbledon in 2010, told the BBC after a mere 2-1/2 hours on court.
"I'm pretty sure Andy will do well at Wimbledon, maybe win this time. I'm really sorry guys, but you will see him winning matches very shortly."
Mahut's second-seeded compatriot Jo-Wilfried Tsonga also overcame a British opponent to go through, beating Jamie Baker 6-3 6-2 in just under an hour.
American Andy Roddick, the seventh seed who was been struggling with injury and was beaten in four sets by Mahut in the first round of the French Open, also went out after losing 6-4 4-6 7-5 to Frenchman Edouard Roger-Vasselin.
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