Kaur announced her decision in a social media post on Tuesday, two weeks after leading India to defend their gold medal at the Asian Games.
"Today, I step down as captain of the Indian Women's Cricket Team across all formats," she wrote in an Instagram post. "This is not an easy decision. It carries years of memories, emotions, sacrifices, and moments that will stay with me for the rest of my life."
The 37-year-old was the Twenty20 captain for more than a decade after taking on the role in 2016, followed by ODI and Test captaincy in 2022. Under her leadership, India reached the semifinals of the 2018 and 2023 T20 World Cups and finished runners-up in the 2020 edition. The pinnacle came last year when India defeated South Africa to win the ICC Women's World Cup on home soil. Earlier this year, Kaur led the team to victory in the Women's Asia Cup and the Asian Games.
Kaur is the first cricketer, male or female, to captain their side in more than 150 T20I matches. She captained India in five Tests, 51 ODIs and 155 T20Is.
According to Indian media, Kaur's decision came a day after she met Devajit Saikia, secretary of the Board of Control for Cricket in India (BCCI), to discuss the future of the women's team.
Opening batter Smriti Mandhana, who has been Kaur's deputy since 2022, is the favourite to take over as captain.
"I leave the captaincy today with a heart full of emotions, but also with peace ... because I genuinely believe my team is in a good place," Kaur said in her post. "Captaincy may end today, but my love for Indian cricket never will. Now, I'm ready to play for the team as a player."