Bopanna and Mergea, seeded sixth, went down 4-6 4-6 to third seeds Ivan Dodig of Croatia and Marcelo Melo of Brazil.
In a lopsided contest, Bopanna and Mergea struggled to handle Dodig and Melo's fine service game.
The Indo-Romanian combine was broken once in the opening set and failed to convert either of the two break points it earned. Bopanna and Mergea also committed a couple of double faults.
The second set followed a similar script and once again, Bopanna and Mergea failed to break their rivals. Dodig and Melo, however, continued to be dominant with their first serve besides converting one of the three break points they earned to outwit the sixth seeds.