The snap election, scheduled for June 3, follows the Constitutional Court of Korea's unanimous decision last week to impeach Yoon over his botched martial law debacle late last year.
Lee Jae-myung, leader of the main opposition Democratic Party (DP), resigned from his post on Wednesday to run in the election.
"I am grateful to have been able to serve as the party leader for three years," he said during a party meeting. He added that he would begin a "new chapter" in his life, hinting at his presidential bid.
Lee, considered a strong contender for the election, is expected to throw his hat into the ring soon.
Former Employment and Labor Minister Kim Moon-soo also declared his candidacy for president the same day.
Having stepped down from his post the previous day, the former labor activist-turned-politician joined an increasingly heated race to select a candidate for the ruling People Power Party, which has no clear favorite despite a flurry of hopefuls including Seoul Mayor Oh Se-hoon, Daegu Mayor Hong Joon-pyo and former party leader Han Dong-hoon.
Kim, who gained sudden popularity during Yoon's impeachment trial among hardline conservatives, claimed he is the only candidate who can defeat Lee.
Meanwhile, the former IT tycoon and perpetual also-ran Ahn Cheol-soo announced yet another presidential bid earlier in the week, while Gyeonggi Province Governor Kim Dong-yeon and Incheon Mayor Yoo Jeong-bok also declared their candidacies.
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