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.
Garcia-Lopez approached the contest on the back of recent success on clay, having won last month’s Grand Prix Hassan II before reaching the quarter-finals at the Monte Carlo Masters.
And the 30-year-old was quick to display encouraging form as he fought back from 3-1 down to break Wawrinka twice and take the first set.
Wawrinka’s pedigree shone through in the second, the Swiss breaking Garcia-Lopez to love in the final game of the set to tie things up.
However, the favourite was unable to build on that momentum and won just two games thereafter as he took his total number of unforced errors to 61.
“It’s an amazing feeling to beat the world number three,” Garcia-Lopez said.
“He’s one of the favourites in the tournament. I played a very consistent and solid game and I’m very happy.
“If you beat the number three in the world then obviously it is pretty special. You have to keep fighting, you just never know.”
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