The Britons, seeded second, lost 7-6 (8-6) 7-6 (16-14) to Brazilian pair Thomaz Bellucci and Andre Sa in front of a partisan home crowd.
Earlier, defending champion Andy Murray won his opening Olympic singles match by beating Serbia’s Viktor Troicki.
But Djokovic, Troicki’s team-mate, is out after a shock loss to Argentina’s Juan Martin del Potro. The world number one lost 7-6 (7-4) 7-6 (7-2) to the London 2012 bronze medalist.
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