Pujara's 153 was studded with 21 fours and he added 222 runs with Virat Kohli for the third wicket.
Pujara reached 150 soon after India crossed the 300-run mark in their second innings.
This is the fourth time that Pujara crossed the 150-run mark in the 16 Test matches that he has played.
In first class cricket, Pujara has scored six double centuries and three triple hundreds.
The day's play started with Pujara and Virat Kohli resuming the Indian second innings.
The third day of the Test was a fantastic one for India and they are firmly in the driving seat.
Zaheer Khan and Ishant Sharma did the job with the ball in the morning session, then Pujara and Kohli batted like champions and by the end of Day 3, India had a commanding 320-run lead with eight wickets in hand.
Ishant and Zaheer took four wickets each to bundle the hosts out, giving only 31 runs in the morning.
Indian opener Shikhar Dhawan was out early but Murali Vijay and Pujara played well after which Jacques Kallis struck to dismiss Vijay.
But Pujara and Kohli played splendidly to pick the right balls and played their shots as the South African bowlers began to tire.
Pujara who was dropped on 51 by Imran Tahir, went on to score his 6th Test century and along with Kohli added 175 runs in the last session of the day to take the Indian lead to the 320-run mark.
With Rohit Sharma, Ajinkya Rahane and captain MS Dhoni to follow, India will look to set South Africa a steep target.
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