Yaya Toure, 43, has signed a three-year contract in the Slovakian capital.
“I’m very happy and excited; honestly, I can’t wait for us to get to work together on Monday," Toure said in a club statement.
"I want to build on that while also bringing something new and unique of my own. Football is everything to me. I love challenges and am incredibly excited to coach a great club with a rich history, a beautiful stadium, and high ambitions."
The Slovan Bratislava job will be Toure's first as the head coach of a senior team after retiring in 2020. Toure has previously worked as an assistant at Olimpik Donetsk in Ukraine, Akhmat Grozny in Russia, Standard Liege in Belgium, and most recently with the Saudi Arabian national team alongside Roberto Mancini, under whose tutelage Toure won the Premier League with Manchester City in 2012.
Club chairman Ivan Kmotrik Jr. called the appointment of Yaya Toure the beginning of a new era for the 24-time Nike Liga winners.
"I am very pleased that Yaya Toure is our new head coach," Smotrik said.
"I am glad we agreed on a three-year contract and that together, we will begin building a new era for Slovan Bratislava. My goal was to bring in someone with the experience at the highest level of world football - and who is also highly motivated to make a name for himself as a coach."
Toure faces a tough start, as Slovan Bratislava will find out their opponent for the Champions League second qualifying round at the draw in Nyon on June 17th.
