The Uruguay striker, who joined Barcelona from Liverpool in 2014, leaves the club having won the Champions League, four La Liga titles and four Copa del Rey trophies.
Atletico Madrid has announced the signing of Barcelona forward Luis Suarez, confirming the Uruguayan striker is set to continue playing in La Liga rather than joining Juventus in Italy.
Barcelona said that Atletico had agreed to pay six million euros for Suarez, who left his last training session in tears on Wednesday having been told over the summer that he was no longer required by new coach Ronald Koeman.
The Uruguay striker, who is Barca's third all-time top scorer with 198 goals in all competitions, had a year left on his contract with the club.
"Atletico Madrid and Barcelona have reached an agreement for the transfer of Luis Suarez, subject to a medical and the formal agreement of a new contract for the Uruguayan striker with our club," Atletico said in their statement.
Suarez to replace Alvaro Morata
Suarez will give a farewell news conference on Thursday.
Barca added: "Barcelona would like to publicly express its gratitude to the player for his commitment and wishes him all the success in the future."
Suarez will replace Alvaro Morata in Atletico's front line after the Spanish striker was loaned to Juventus for a season with an option to buy.
Since joining Barca from Liverpool in 2014, Suarez has won a host of trophies, including the 2015 Champions League and four Liga titles.
He leaves as the club's third highest scorer with 198 goals behind Cesar Rodriguez (232) and Lionel Messi (634).
Bid to get an Italian passport
The move to Barcelona's La Liga rivals follows a failed attempt to join Juventus.
Juve coach Andrea Pirlo disclosed last week a deal was unlikely because of delays in the Uruguayan's bid to get an Italian passport.
On Tuesday, prosecutors in Perugia said they suspected Suarez of cheating to pass his Italian language test with the aid of examiners suspected of helping him.
The exit of the 33-year-old from Camp Nou comes as Koeman attempts to reshape Barcelona.
As well as Suarez, the Dutchman has shown the exit to Arturo Vidal and Ivan Rakitic, while French defender Samuel Umtiti is also set to leave.
Spanish television channel Gol showed Suarez wiping away tears with his sleeve as he drove off after saying his last goodbyes to teammates at Barcelona's Sant Joan Despi training centre.