Ably supported by Steve Smith and his unbeaten 65, Head blitzed India's bowling attack in a dominant middle session on Sunday in which Australia added 130 runs.
As he and Smith took their partnership to 159 by tea, the flamboyant left-hander regularly upper-cut India's quicks to the third-man boundary, picking out the gaps in the field and hammering the ropes.
He brought up his century just before tea to go to the break unbeaten on 103, with his last 42 runs coming from only 30 balls.
Steve Smith made a composed half-century while Head went on the attack. (Jono Searle/AAP PHOTOS)
After heavy rain wiped out most of day one, India appeared to be slightly on top when Jasprit Bumrah struck twice early on Sunday and Australia fell to 3-75.
But Head quickly obliterated that advantage, in what could be a crucial innings in this Border-Gavaskar Trophy with the five-match series locked at 1-1.
He has struck 13 boundaries in his knock, bringing up his ninth Test hundred off 115 balls and continuing his run of dominance over India after last week's equally-crucial century in Adelaide.
Head made his intent known early when he slapped Nitish Kumar Reddy for four, and soon afterwards drove Bumrah for another boundary.
The left-hander then took great joy in punishing India any time they went short or offered width, with seven of his boundaries coming on the cut or upper cut.
Spinner Ravindra Jadeja was also hit for two straight boundaries down the ground, while Head's shot of the day was a superb hook shot off Mohammed Siraj.
Head's ton was his third in four Tests against India, after Adelaide last week and last year's Test Championship final at The Oval.
Marnus Labuschagne departs after his 55-ball innings. (Jono Searle/AAP PHOTOS)
Head's attacking brilliance allowed Smith to play at his own pace down the other end, in his first half-century in five Tests.
The vice-captain survived an lbw review on umpire's call when he left a Siraj ball before lunch, while another inside-edge off Bumrah narrowly missed the stumps.
Otherwise the 35-year-old looked composed, driving nicely and picking off runs through the leg side.
He played one of the shots of the day when he drove Akash Deep back down the ground to the boundary, while also producing dominant cuts and pulls against Reddy.
The veteran had earlier steadied the ship after Bumrah edged out Usman Khawaja (21) and Nathan McSweeney (9) early, before Marnus Labuschagne was also caught at slip driving hard at Reddy on 12.