Strategy Analytics said Android grabbed 65.8% of global tablet sales in the first quarter, up from 53% a year ago.
Apple meanwhile saw iPad sales slump and its market share tumbled to 28.4% from 40.3% a year earlier, the survey showed.
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"Android continues to make steady progress and now commands two-thirds of the tablet market share," said Peter King, analyst at Strategy Analytics.
While Apple ignited the tablet market with its first iPads, it has now lost its dominance to Android in the same manner as the iPhone has seen its share eroded in the smartphone market.
The report said iPad sales were down 16% from the same period a year ago.
"We believe that the disappointing performance in the early part of the calendar year is because Apple has changed its product release cycle to the holiday timeframe," King said.
He added that Apple "will likely lose share over the next several months to refreshed Android products, but we believe Apple will win back meaningful high-end market share during the final months of the calendar year."
Android sales totaled some 38 million in the period to Apple's 25.6 million, the report said.
The survey also found a steady market share for tablets using Microsoft Windows.
Windows tablet sales rose to 3.4 million from 2.8 million a year earlier, keeping a steady market share of 5.8%, according to Strategy Analytics.
"There may be an uptick in Windows following Microsoft's decision to offer Windows for free for sub nine-inch devices," the report noted.
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