De Villiers had just got off the mark, added three runs to his side's cause when Mishra showed him the way back.
It was an easy catch for Ishant Sharma at mid-off to dismiss the visitors' fourth wicket of the innings in Ashwell Prince off Harbhajan.
Hashim Amla held the fort and led South Africa past the 150-run mark as India stepped on the gas to stake claim for a victory.
Amla completed a patient half-century after South Africa had resumed the day's proceedings from an overnight 115/3.
Amit Mishra and Harbhajan Singh had put India on course for victory on a rain-hit fourth day in Kolkata.
Mishra claimed Graeme Smith (20) in a morning session at the Eden Gardens which was shortened to an hour due to a wet outfield and the spinner struck again in the afternoon to secure Jacques Kallis' (20) scalp, Harbhajan Singh removing Alviro Petersen (21) in between to leave the home side on course for a series-levelling win.
Rain and Hashim Amla (49 not out) were hurdles to more success for the home side as the Proteas ended the day on 115 for three, still 232 runs behind India's first innings score.
The start to the morning session on the fourth day was delayed by more than 90 minutes, but Smith and Petersen had made a determined start once play resumed.
South Africa trail by 175 runs
South Africa 172/6(74.0 overs)
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