Pujara's innings and his last-wicket stand of 46 runs with Jasprit Bumrah (6) have virtually made the encounter at Rose Bowl a game of second innings.
He got to his 15th century, and second outside Asia, with a double over the bowler's head, and well aware of the significance of the knock to the final outcome, the unassuming India number three raised his bat and helmet in celebration.
It was appropriate, even as the visitors inched closer to England's first-innings effort.
Pujara's footwork against spin, always a feature of his game in home conditions, came to the fore in the first innings of an overseas Test, and it helped India. As he settled down, the batsman looked comfortable against the pacers and ensured there was no hiccup from at least one end.
In what turned out to be another eventful day of Test cricket, India slumped from 161 for four to 195 for eight in the final session of play, with veteran off-spinner Moeen Ali doing the bulk of damage.
Had it not been for Mooen's impressive return of 5/63, India would have run away with the game as the visitors negated the seam duo of James Anderson and Stuart Broad in the first session, reaching 100 for two at lunch.
England enjoyed upper hand in the post-lunch session despite dogged defiance from Pujara as India went into tea at 181 for five.
Rishabh Pant (0) patiently left the deliveries outside the off-stump before Moeen Ali got one to straighten and trapped him leg-before at stroke of tea.
Pujara, however, batted in his customary style, reaching 70 off 151 balls with nine boundaries to his credit.
Pujara took time to settle down and waited patiently for the loose deliveries to dispatch them to the boundary.
Skipper Virat Kohli (46) once again looked good for a big score before Sam Curran managed to draw him forward, inducing a thickish outside edge to Alastair Cook in the slip cordon.
Kohli and Pujara added 92 runs for the third wicket after Shikhar Dhawan (23) and Lokesh Rahul (19) were dismissed cheaply by Stuart Broad (2/50).
Kohli's 71-ball knock had six boundaries.
However, vice-captain Ajinkya Rahane (11) would consider himself unlucky as he was trapped leg before off a no-ball from Ben Stokes. The TV replays clearly showed that Stokes had overstepped but a howler from third umpire Joel Wilson proved to be Rahane's undoing.
Despite calling for a review, Wilson, after repeated replays, ruled it as a legal delivery.
Earlier, starting from overnight 19 for no loss, Dhawan and Rahul made a sedate start. The duo were watchful for any hint of lateral movement, similar to what the Indian pacers generated on the first morning of the match.
James Anderson (0-37) didn't find much movement, while Stuart Broad (2-34) did hit on a troubling length to the left-handed Dhawan whenever he pitched the ball up.
Broad struck in the fourth over of the morning, trapping Rahul lbw in the eighth over of the innings. The batsman opted for DRS, but the decision stayed in England's favour.
The pacer had another appeal against Dhawan turned down, this time for caught behind in the 14th over, and even on DRS, the batsman benefitted as the ball only clipped his thigh pad.
Bowling a lengthy first spell this morning, Broad finally got a second reward for his efforts as he continued to tease Dhawan outside the off-stump. Finally, the edge came in the 18th over, with the batsman caught behind immediately after India crossed 50.
It brought Pujara and Kohli together at the crease, and thanks to the latter, the Indian run-rate picked up once again. Kohli hit four fours during his 40-ball stay thus far, and in doing so crossed 6000 runs in Test cricket, the second-quickest Indian batsman after Sunil Gavaskar to reach the mark.
England's desperation could be seen in that they put both spinner Adil Rashid (0-5) and Moeen Ali (0-0) into the attack just before lunch. Sam Curran (0-16) had earlier toiled hard but in vain, and even Keaton Jennings (0-4) was tried for two overs.
Pujara and Kohli though settled down for what should be a lengthy Indian innings in helpful batting conditions, as the score crossed 100 at the stroke of lunch.
The Indian pacers rattled England and reduced them to 86 for six, before Sam Curran's second Test half-century helped them post 246 runs in the first innings.
England lead the five-match series 2-1, after winning the first two Tests at Birmingham and Lord's, with India pulling one back with victory in Nottingham.
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