In 2021, Barty started to partner with Jennifer Brady. They were not able to play many tournaments during the first half of the year, as they had to withdrew from both the Australian Open and the French Open due to injuries, but managed to win the title in Stuttgart. This was Brady's maiden doubles title, and Barty's first one since 2019. At the 2020 Olympics, Barty partnered Storm Sanders in the women's doubles and reached the quarterfinals, where they were beaten by top-seeded Krejčíková and Katerina Siniakova, and fellow Grand Slam champion John Peers in the mixed doubles, where they went on to become bronze medalists.