It was the 27-year-old Russian's fifth Grand Slam title, bringing her level with Martina Hingis on the all-time list and it came 10 years after she won her first major at Wimbledon 2004.
Sharapova, who completed a career sweep of all four Grand Slam titles in Paris in 2012 before losing to Serena Williams last year, also moved to number two on the all-time prize money earnings, with only the American ahead of her.
"It's the toughest Grand Slam final I have ever played," said Sharapova.
"I can't believe that at 27 I have won the French Open more times than any other Grand Slam."
The consolation for Halep, whose meteoric rise to the top bracket in women's tennis over the last 18 months has projected her as a potential champion, was that she will climb to a career-high third in the world rankings.
Fourth-seeded Halep did not drop a single set in her six matches, while seventh-seed Sharapova needed to battle back from first set losses in her three previous outings.
But experience was massively on the Russian's side. This was her ninth Grand Slam final dating back 10 years, while Halep was playing in her first at the age of 22.
Sharapova also towered over her opponent at 1.88 metres (6 feet 2 inches) compared to Halep's 1.68 metres (5 feet six inches).
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