The 32-year-old Italian crammed seven birdies in a flawless seven-under-par effort at Wentworth while world number one Rory McIlroy could only manage a 71 on a day of unbroken sunshine on the outskirts of London.
Swede Robert Karlsson was in second place on 67, one ahead of Spanish pair Miguel Angel Jimenez and Jorge Campillo, British duo Marc Warren and Chris Wood and 2009 U.S. PGA Championship winner YE Yang.
It was world number 66 Molinari, though, who was head and shoulders above everyone else and his performance strengthened the depth of feeling he has for the European Tour's flagship event.
"I love this place," the former Ryder Cup player told reporters. "I've played very well here the last few years and it's very good to be back.
"I think I missed only one green. It rewards accuracy more than others so it suits my game."
Molinari has finished in the top 10 here for the last three years and is hoping another good week can help him get back in the world's top 50.
"It's a great start but unfortunately nothing more than that," said the 2012 Spanish Open champion. "We don't get the trophy on the first day so I need to keep my head down and do the same tomorrow and Saturday and Sunday."
His older brother Edoardo will definitely not be around for the remainder of the week after he was forced to pull out with a wrist injury on the 17th hole.
HARRINGTON OUT
Triple major winner Padraig Harrington also had to withdraw on the third hole because of a sore shoulder.
For McIlroy, it was a day of treading water and he showed his annoyance with the occasional flash of indiscipline.
The defending champion tossed his club across the fairway in frustration after playing an errant second at the par-five 17th.
"I felt myself getting a bit angry out there which I haven't been doing the last few weeks," said McIlroy.
"I just need to stay in control of my emotions because I feel like ... if I'm a little tired or a little fatigued mentally I'll start to be hard on myself.
"I feel like my patience was sort of wearing thin out there today so I just need to try and stay a little bit more patient."
McIlroy, who lost his cool when he hurled a club into a water hazard at the WGC-Cadillac Championship in Florida in March, is playing in his fourth tournament in a row this week, an untypically busy schedule for the 26-year-old.
World number six Justin Rose also began his campaign with a 71 while U.S. Open champion Martin Kaymer had to settle for a 72.
Andrew Johnston won a car from the sponsors after recording a hole-in-one at the 10th but fellow Briton Craig Lee was not so lucky because there was no prize on offer for his ace at the second.
(Editing by Justin Palmer)
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