Mannarino made his Grand Slam singles debut at the 2007 French Open, where as a wild card, he lost in the first qualifying round to Marin Čilić in straight sets.
Mannarino received a wild card for the singles main draw of his home Grand Slam tournament, the 2008 French Open, where he lost to Argentine qualifier Diego Junqueira in the first round in straight sets. He also received a wild card for the 2008 French Open men's doubles (it was his Grand Slam men's doubles debut), losing in the first round.
Mannarino played at the 2008 Open de Moselle in France, entering the singles main draw as a qualifier; he reached the semifinals, defeating sixth seed Andreas Seppi in the first round, Rik de Voest in the second round, Marc Gicquel in the quarterfinals, before losing to Paul-Henri Mathieu in the semifinals in two tiebreaks. As a wild card, he lost in the main draw singles first round of the 2008 Paris Masters to Dmitry Tursunov. In November 2008, he played in an ATP Challenger Tour tournament in Jersey, where, seeded fourth, he won the singles event, defeating Andreas Beck in two tiebreaks in the final. He participated in the inaugural Masters France in December 2008, an exhibition tournament, along with a number of top French players, but lost his three round-robin matches in straight sets to Paul-Henri Mathieu, Michaël Llodra and Arnaud Clément.
He received a main draw singles wild card for the 2009 Australian Open, where he lost to 14th seed Fernando Verdasco in the first round.
In 2011, he lost in the main draw singles second round of the Australian Open and Wimbledon, falling to six-time champion Roger Federer in the latter in straight sets.
At the 2013 Wimbledon Championships, Mannarino beat Pablo Andújar in the first round, losing only six games. He then reached the singles third round of a Grand Slam for the first time, after his second round opponent John Isner was forced to retire at 1-1 in the first set due to a knee injury. He then beat qualifier Dustin Brown, who had just beaten Lleyton Hewitt to reach the fourth round. He pushed veteran Łukasz Kubot to five sets in his fourth-round match, but ultimately lost, setting up an all-Polish quarterfinal between Kubot and up-and-coming player Jerzy Janowicz.
At the 2015 Miami Open, Mannarino was the 28th seed and thus received a bye into the second round where he defeated Albert Ramos Viñolas. He beat 7th seed and the 2014 Australian Open singles champion Stanislas Wawrinka in the third round but lost to unseeded Dominic Thiem in three sets in the fourth round.
At the 2016 Australian Open, the unseeded pair of Mannarino and Lucas Pouille defeated three seeded pairs (including the top-seeded pair of Horia Tecău and Jean-Julien Rojer in the quarterfinals) to reach the semifinals, where they lost to Jamie Murray and Bruno Soares.
The unseeded Mannarino reached his third career ATP World Tour singles final at the 2017 Antalya Open; he defeated two seeded players Borna Ćorić (in the first round) and Fernando Verdasco (in the quarterfinals) to advance to the final, where he lost to Yūichi Sugita in straight sets. At the Wimbledon Championships one week later, Mannarino upset no. 19 seed Feliciano López in the first round and no. 15 seed Gaël Monfils in the third round before losing to no. 2 seed Novak Djokovic in the fourth round. He reached his first career ATP World Tour Masters 1000 singles quarterfinal at the 2017 Rogers Cup, where he upset no. 6 seed and world no. 10 Milos Raonic in the second round before losing to Denis Shapovalov in the quarterfinals. The unseeded Mannarino defeated top seed and world no. 5 Marin Čilić (the biggest singles win of his career and his first career win over a member of the Top 5 in the ATP singles rankings) in the semifinals of the Japan Open to reach his first career ATP World Tour 500 Series singles final, where he lost to fourth-seeded David Goffin. In October, Mannarino reached his third ATP World Tour singles semi-final of 2017 at the Kremlin Cup, where he lost to Ričardas Berankis. The following week, the 7th seeded Mannarino lost in the quarterfinals of the Swiss Indoors to top seed Roger Federer in three sets.
Mannarino played his first ATP World Tour tournament of 2018 at the Sydney International, where he lost in the quarterfinals to Fabio Fognini. Seeded no. 26, Mannarino reached the singles main draw third round of the Australian Open for the first time in his career, where he lost to no. 5 seed Dominic Thiem in straight sets. On January 29, Mannarino reached his then career-high of world no. 25 in the ATP singles rankings. Mannarino made his Davis Cup debut in the 2018 Davis Cup World Group first round tie against the Netherlands, replacing Lucas Pouille who had withdrawn a few hours before the start of his first singles match on 2 February against Thiemo de Bakker because of torticollis. Mannarino lost his first singles match against Thiemo de Bakker (who was world no. 369 in the ATP singles rankings) in three sets but won his second singles match against Robin Haase in five sets to give the French an unassailable lead against the Dutch.
In the first week of February, the second-seeded Mannarino was upset by the unseeded Marcos Baghdatis in three sets in the second round of the Sofia Open. One week later, the fourth-seeded Mannarino lost in the semifinals of the New York Open to the no. 2 seed Sam Querrey in three tight sets. Mannarino lost before the quarter-final round of the singles main draw of his next four ATP World Tour tournaments in Acapulco, Indian Wells, Miami and Monte-Carlo. At the Barcelona Open, the 11th-seeded Mannarino held three match points in the final set of his third round match against the 5th-seeded Pablo Carreño Busta before losing in a tight tie-break.
He won his first ATP Tour singles title in 2019 in Rosmalen on grass (he defeated Jordan Thompson in the final). He was the singles runner-up at six ATP Tour tournaments held in Auckland, Bogotá, Antalya (2017), Tokyo, Antalya (2018) and Moscow. Mannarino has achieved victories over four players ranked in the Top 10 of the ATP singles rankings; Marin Čilić, Milos Raonic, Jo-Wilfried Tsonga and Stan Wawrinka.
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