The 27-year-old has signed a five-year contract, with the fee reported by Benfica in Portugal to be six million euros ($8.16 million).
Garay, a member of Argentina's squad for the World Cup finals in Brazil, began his career with Newell's Old Boys in 2004 before joining Racing Santander in Spain, where he spent two and a half seasons.
He moved to Real Madrid in 2008, although he was immediately sent back on loan to Racing. When he returned to Real, he played 31 matches in La Liga and scored one goal.
After joining Benfica he become one of the team's key players. He won four trophies in Lisbon, including last season's Portuguese league title, and appeared in two Europa League finals.
"I want to thank everyone who supported me in these three magical years I spent at Benfica, in particular the president, who believed and invested in me, and the coach, who made me evolve and reach a level that I am proud of," Garay told the Benfica website (www.slbenfica.pt)
Garay won his 21st cap for his country as Argentina took on Nigeria in World Cup Group F on Wednesday.
He will be the second Argentinian on Zenit's books, alongside left back Cristian Ansaldi.
($1 = 0.7355 Euros)
(Editing by Stephen Wood)
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