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The fifth-wicket pair took their overnight stand to 256, a South Africa record for any wicket against India who were out for 76 in the opening session of the match.
The visitors, looking for an Asian treble following successes in Pakistan and Bangladesh, were 494 for seven -- a commanding lead of 418 -- when rain brought an early end on day two.
The opening match of the three-Test series ended in a high-scoring draw in Chennai last week.
De Villiers, who struck 17 fours and two sixes in his remarkable innings of 217, also shared in a 66-run stand for the sixth wicket with Mark Boucher (21).
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