Harris, who entered the tournament ranked 40th in the world, lost 4-6, 7-6 (7/5), 1-6 to world No 57 Marton Fucsovics.
The Hungarian star triumphed in the match which lasted two hours and 35 minutes.
Harris was coming off his best ever performance at a Masters 1000 event when he reached the last 16 at last month’s Miami Open.
Lloyd Harris will be looking to improve ahead of the French Open
That performance was good enough to see the 25-year-old move up four spots in the rankings – and above Swiss great Roger Federer.
Harris will be looking for an improvement in the coming weeks in Madrid and Rome ahead of the year’s second Grand Slam, the French Open at Roland Garros, which gets underway on Sunday, 22 May.
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