Dhoni's previous best Test score was 148 against Pakistan.
Australian pacer Moises Henriques bowled out Harbhajan Singh to give India eighth blow at the score of 406.
India lost their seventh wicket when R Ashwin edged a Nathan Lyon delivery onto his stumps.
Tea report
Virat Kohli smashed his fourth Test hundred, while skipper Mahendra Singh Dhoni inched closer to his sixth as India reached 371 for six at tea.
Also notable was the magnificent half-century by Sachin Tendulkar (81).
At the break, Dhoni was holding fort with R Ashwin (3) giving him company.
India scored at a decent pace to be 263 for four at lunch, but after the break, the innings accelerated with Kohli and Dhoni breaking free against an attack that, despite asking a few questions, never looked very threatening.
Kohli eventually fell to Nathan Lyon, who was rewarded for his perseverance after grabbing Tendulkar's wicket in the morning session.
However, the breakthrough came only after Kohli and Dhoni had put on 128 runs for the fifth wicket and that too at rapid a pace.
The two were together for 26.1 overs and plundered 54 runs off the first seven overs with the new ball that was taken in the 83rd over.
Australian skipper Michael Clarke shuffled his bowling resources and even bowled himself but the home batsmen remained fluent in their stroke-making, entertaining the large Sunday crowd that turned up at the M A Chidambaram Stadium.
India's 300 was up in 87 overs but a couple of overs later, the team lost Kohli's wicket to a rather casual shot.
Trying to go over mid-on, Kohli failed to get the elevation and ended up holing out to Mitchell Starc. His superb knock included 15 fours and a six.
Kohli's departure, however, did not affect Dhoni, who went about his job with ease. The only time he seemed in trouble was in the 95th over when he survived a run out chance after a mix-up with Ravindra Jadeja.
The Indian skipper called for a single but backed out twice after seeing Phillip Hughes dive for the ball at midwicket. But Dhoni eventually risked the run after Hughes failed to collect the ball cleanly.
Earlier, in the morning session, Tendulkar missed out on a century but India scored at a brisk pace. The veteran was the only Indian to be dismissed in the first session but scoring remained unaffected as Dhoni and Kohli dropped anchor to put the home side in a comfortable position.
Clarke opened the bowling with tearaway pacer James Pattinson, who had taken all three of the Indian wickets to fall yesterday, hoping to get a quick breakthrough.
Pattinson bowled five overs in his first spell, gave away just six runs and asked quite a few questions from the set batsmen but could not get a wicket.
He completed 23 overs but managed to add just one wicket to the three wickets he picked up yesterday. That wicket was of Jadeja, who ran out of luck after 16 runs to the total.
Similar was the case of Peter Siddle, who was economical but unlike Pattinson, could not get a single wicket.
After Pattinson and Siddle could not get a wicket in their opening spells, Clarke changed the bowlers on both the ends, bringing in off-spinner Lyon and seamer Starc.
Lyon, against whom Tendulkar had survived a close leg-before shout yesterday, delivered when he dismissed the well-set veteran.
Tendulkar was on 81 and looked good for a hundred but Lyon denied him the milestone. The Australian tossed a delivery outside the off-stump in the 64th over which took a faint inside edge from Tendulkar's bat before spinning through to the stumps.
Tendulkar faced 159 deliveries during the knock, which was laced with seven fours. The right-hander had shared a 91-run stand with Kohli during his stay at the crease.
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