The German, who joined the tournament on a late wildcard, was beaten 3-6 7-5 7-6 by lucky loser Nicolas Jarry.German world number three Zverev, who is looking to improve on his disappointing start to 2019, came back from a double break down in the third set but blew a match point at 6-5.
It was the biggest win of the Chilean Jarry's career. The world number 81 will now face either Grigor Dimitrov or Fernando Verdasco in Thursday's third round. Zverev's brother Mischa Zverev was also eliminated, going out 6-3 6-1 to David Ferrer in the first round, while Kei Nishikori eased to a 7-5 6-2 win over Taylor Fritz to secure a place in the third round.
Top seed and world number two Rafa Nadal begins his campaign to win the Barcelona Open for a record 12th time on Wednesday against Leonardo Mayer.
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