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Francisco Cerúndolo reached his first ATP tour final at the 2021 Argentina Open as a qualifier but was defeated by world No. 9 Diego Schwartzman. He was the first qualifier to reach the final in Buenos Aires since José Acasuso in 2001. At the time, Acasuso was coached by Cerúndolo's father, Alejandro Cerúndolo.
Cerúndolo recorded his first ATP Tour victories on hard court at the Masters 1000 event in Miami, defeating Tallon Griekspoor and seeded players Reilly Opelka and Gael Monfils en route to the fourth round. He beat Frances Tiafoe in the fourth round to advance to the quarterfinals. He advanced to the semifinals after Jannik Sinner retired during their match due to foot blisters. Ranked World No. 103 at the time, he became the lowest-ranked semifinalist in the history of the Miami Open, and also became the first male player since Jerzy Janowicz in 2012 to reach the semifinals on their Masters 1000 level debut. He lost to 6th seed Casper Ruud in the semifinals in straight sets. Following this result, his ranking rose 52 places to a career high of World No. 51.
His younger brother Juan Manuel Cerúndolo (born 2001) is also a tennis player. Juan Manuel was also in his first final and won his first title at the 2021 Córdoba Open one week before his brother's final.
The Cerúndolos became the first brothers to reach consecutive finals on the ATP Tour since 2017, when Alexander Zverev won the title in Rome and Mischa Zverev reached the final in Geneva. In Cordoba, Francisco contested the first ATP Tour event in which his brother was also competing, making them the first Argentine brothers in 40 years to appear in the same tournament.