In January 2007, Di María had an opportunity to play in the Russian Premier League when Rubin Kazan offered him a contract. At first, he agreed, but soon afterwards, he changed his mind and turned down the offer.

On August 23, 2008 he had the perhaps best moment of his career so far. He scored the game-winner, a chip over the keeper from the edge of the area, in Argentina's 1-0 victory against Nigeria to capture their second straight Olympic Gold Medal in the final game of the Olympic tournament.

On February 27, 2010, di María scored his first hat trick in a classic 4-0 win against Leixões.