The world number three won the Australian Open back in January, but was outclassed on Court Philippe Chatrier by Garcia-Lopez, who ultimately cantered to a 6-4 5-7 6-2 6-0 victory.
Wawrinka looked to have recovered from losing the first set when he levelled the match by taking the second.
However, Garcia-Lopez stormed through the final two sets to ensure his opponent became the first Australian Open winner since Petr Korda in 1998 to lose in the first round at Roland Garros.
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