Herbert won the Wimbledon boys' doubles title with partner Kevin Krawietz in 2009, beating French duo of Julien Obry and Adrien Puget in the final.

He also reached the 2009 US Open boys' singles semifinals, where he lost to eventual champion Bernard Tomic of Australia.

He then made it through three rounds of qualifying, beating Borna Ćorić, Daniel Kosakowski and Miloslav Mečíř Jr. to make the main draw at 2014 Wimbledon for the first time.

Herbert got his fifth career main draw win at the ATP Tour level at the Swiss Indoors in Basel, beating Édouard Roger-Vasselin in a tight three-setter to set up a clash with 14-time Grand Slam winner Rafael Nadal, his first meeting with a Major champion and former world number 1.

Herbert again battled through three rounds of qualifying, beating Hans Podlipnik Castillo, Facundo Argüello and Íñigo Cervantes (the latter over five sets) to make the main draw of Wimbledon.

In the first round he beat Hyeon Chung in a three-hour, five-set match, clinching the final set 10–8, claiming his first win in the main draw of a grand slam.

In the second round, he lost in straight sets to Bernard Tomic, the player who had beaten him in the semi-finals of Junior US Open in 2009.

In doubles, Herbert reached two Grand Slam finals alongside fellow Frenchman Nicolas Mahut.

Herbert and Nicolas Mahut won three ATP World Tour Masters 1000 doubles titles in a row in the first half of 2016, in Indian Wells, Miami, and Monte Carlo.

At the 2016 Wimbledon Championships, Herbert and Mahut beat Julien Benneteau and Édouard Roger-Vasselin in the all-French final to win their second grand slam tournament as a team.

Herbert and doubles partner Nicolas Mahut won their first title of 2017 together at the Rome Masters defeating Ivan Dodig and Marcel Granollers.

[17] In Doha, Herbert's first tournament of the year, he recorded his second top-ten win against Dominic Thiem, before falling to Tomáš Berdych in the quarterfinals.

36 on 11 February 2019 after he reached his third ATP tour final at the 2019 Open Sud de France in Montpellier, where he fell to countryman Jo-Wilfred Tsonga.

[23] In the 2019 clay season in Monte-Carlo Herbert captured his third top 10 win against Kei Nishikori to reach the third round.

[25] Herbert reunited with Nicolas Mahut to play the Paris Rolex Masters which they won defeating Karen Khachanov and Andrey Rublev in the final.

[26] The pair qualified for the ATP finals for the 5th straight year,[27] where they went undefeated in the round robin stage, and then went on to lift the trophy, without dropping a set throughout the tournament.

[45] Getting past qualifying at the Madrid Open, he lost in the first round to Spaniard Alejandro Davidovich Fokina in three sets.

[48] At the second Grand Slam of the year, the French Open, he pushed 18th seed Jannik Sinner to five sets, but he ended up losing their first-round match.

The home favorites saved three match points en route to the final defeating second seeds Juan Sebastián Cabal/Robert Farah.

[63] At the 2023 Moselle Open in Metz he recorded his 100th singles career win over Luca Van Assche to reach the semifinals.

[66][67] Playing with Albano Olivetti, Herbert was runner-up at the 2024 Moselle Open, losing to Sander Arends and Luke Johnson in the final.