The fifth seeded Indo-Zimbabwean pair lost 7-5, 1-6, 8-10 to the Taipei-Chinese team in one hour and 30 minutes in the euro 3,671,405 clay court tournament.
There was not much to separate the two pairs as the Portugal Open winners won 62 points to 67 of their top seeded rivals.
Sania and Cara converted four break chances while Hsieh and Peng broke them five times in the match which was decided via a thrilling Super Tie-Breaker.
Sania and Cara split euro 27,270 as prize money and earned 215 ranking points each.
Indian challenge is still alive in the tournament as Rohan Bopanna and his Pakistani partner Aisam-ul-Haq Qureshi, seeded eighth, have been given a bye in the first round of the men's doubles.
They face Italian Andreas Seppi and big serving Canadian Milas Raonic in the pre-quarterfinals.
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