The hosts were ahead of the visitors by 244 runs with five second innings wickets in hand.
The home batsmen, who were dismissed in their second essay were first innings and series top-scorer Murali Vijay (5), his opening partner Shikhar Dhawan (39), one-down Cheteshwar Pujara (31), captain Virat Kohli (16) and Ajinkya Rahane (9).
At the break, Rohit Sharma and wicket-keeper Wriddhiman Saha were unbeaten without any runs to their name.
With the visitors on a shaky 11 for 2 overnight in reply to the home team's modest first innings tally of 215, expectations were high that the Indian spinners would create mayhem on a venomous VCA Stadium track.
True to predictions, Ravichandran Ashwin (5 for 32), Ravindra Jadeja (4 for 33) and Amit Mishra (1 for 9) combined forces to slice through the nervous Proteas' batting order and shoot them out for their 12th lowest Test score and their worst since readmission to international cricket in the early 1990s.
The total innings beat the previous low of 84 against India made in Johannesburg in December 2006 as well as the previous lowest in this country of 105 in November 1996.
None of the Proteas' batsmen, barring to some extent left handed Jean-Paul Duminy - who top-scored with 35 in 65 balls after being let-off twice - showed inclination or skill to counter the threat posed by Ashwin and Jadeja.
Off-spinner Ashwin bowled unchanged for 16.1 overs from the end opposite to the pavilion to return with his 14th five-wicket haul in an innings in his 31st game.
(REOPENS DEL 20)
Left-arm spinner Jadeja was not too far behind and sent back dangerman A B de Villiers for a duck, Faf du Plessis and Dane Vilas today to add to his kitty that already had Imran Tahir yesterday.
The deliveries that got rid of de Villiers and du Plessis were classy ones, the first one stopping and deceiving the batsman who put up a return catch and the second turning across the face of the bat and clean-bowling du Plessis.
Leg-spinner Amit Mishra, brought into the attack late in the pre-lunch session, got rid of the stubborn Duminy who was let off by Indian skipper Virat Kohli and wicketkeeper Wridhiman Saha, both off Ashwin's bowling earlier.
India went to lunch at 7 for no loss in four overs but then lost Vijay. Dhawan and Cheteshwar Pujara (31) then added 44 runs to help India cross the 50 mark.
Pujara looked in good touch by hitting Kagiso Rabada and Duminy for fours in successive deliveries before the latter deceived him with an arm ball that crashed into the off stump as the batsman played for the turn.
Not to be left behind, Rahane departed at the stroke of tea while trying to slog Tahir's googly to be caught off the leading edge by a diving Duminy at backward point.
Tahir's figures were a very impressive 4-1-8-3 at the end of the second session in which the hosts added 101 runs in 27 overs and lost their top five batsmen.
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