With nearly 90% of the vote counted, leftist Michelle Bachelet had 62% to 38% for Evelyn Matthei, a former minister from the ruling centre-right coalition.
Michelle Bachelet first served as president between 2006 and 2010, after which she was obliged by electoral laws to stand down.
She narrowly missed out on outright victory in the first round last month.
“I am happy with the result and victory and I shall be a president for everyone in Chile,” Michelle Bachelet, 62, said as she received a congratulatory telephone call from outgoing President Sebastian Pinera, according to Reuters.
At a speech to supporters, Michelle Bachelet said: “I am proud to be your president-elect today. I am proud of the country we’ve built but I am even more proud of the country we will build.”
She is now set to become the first leader in Chile to serve two terms since the military rule of General Augusto Pinochet in 1973 to 1990.
Upon hearing the news, her supporters have been celebrating on the streets by waving flags and sounding car horns in the capital Santiago.
“It is clear at this point. She won. And we congratulate her. Later on, I will go speak with her personally,” Evelyn Matthei, 60, told reporters.
Official results of Sunday’s run-off are expected soon. Turnout appears to have been lower than expected.
A pediatrician by training, Michelle Bachelet won 47% of the vote in the first round on November 17. Evelyn Matthei secured 25%.
Michelle Bachelet leads an alliance of her Socialist Party, Christian Democrats and Communists and has campaigned on policies designed to reduce the gap between rich and poor.
Chile is one of the richest countries in Latin America, but millions have staged protests over the past few years to push for a wider distribution of wealth and better education.
Michelle Bachelet wants to increase taxes to offer free university education and reform political and economic structures dating from the dictatorship of Gen. Augusto Pinochet.
Evelyn Matthei, 60, entered the race after two candidates of the centre-right alliance resigned earlier this year – one for alleged financial irregularities, the other one after struggling with depression. She has called for a continuation of the policies of outgoing President Sebastian Pinera, asserting that Chileans are “better off” now than when he came to power four years ago.
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