The world number seven recovered from an error-strewn first set to win 3-6, 7-5, 6-3, making up for her disappointment in losing the 2000 final to Venus Williams.
Dementieva clenched her fists in celebration and then wiped away tears of joy after stopping the in-form Safina for the first time in four attempts this year.
"It's very difficult to explain the way I feel right now. It will take a few days before I realise I'm Olympic champion," Dementieva said.
"But this is for sure the biggest moment in my career, in my life. I will never forget this moment."
Russia had already been guaranteed the first tennis podium sweep in 100 years when Vera Zvonareva, a late call-up for the injured Maria Sharapova, clinched the bronze medal play-off against China's Li Na 6-0, 7-5.
"Having three Russian girls left standing in the Olympics is a huge moment for Russia," Dementieva said.
"I know we were expecting and planning for some medals but I don't think anyone could expect three medals from the girls. So this is really big moment for Russia."
It was the first one-two-three in any tennis event since 1908, when Great Britain also collected all three women's singles medals.
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