In June 2013, Smitková made her WTA Tour main-draw debut at the Nürnberger Versicherungscup.

In the Wimbledon qualifying in June 2014, Smitková again reached the third round,[4] this time defeating Madison Brengle in three sets to seal her maiden Grand Slam main-draw appearance.

In the main draw, she defeated Hsieh Su-wei in the first round before upsetting grass-court specialist CoCo Vandeweghe, who was ranked world No.

[5] Her run was over in round four, after losing to fellow Czech Lucie Šafářová in straight sets.

[6] Only main-draw results in WTA Tour, Grand Slam tournaments, Fed Cup/Billie Jean King Cup and Olympic Games are included in win–loss records.