Head was brutal at times as he scored 112 in 84 balls while Cooper Connolly struck 78 and opener, and stand-in captain, Mitchell Marsh hit 53 as the tourists piled on 356-6 in their 50 overs after being sent in to bat the toss by home skipper Sikandar Raza.
Marsh and Head put on 130 for the opening partnership before the stand was broken in the 19th over by left-arm spinner Wellington Masakadza, but Connolly kept up the aggressive tempo as his runs came off just 69 deliveries.
There were contributions of 21 from Josh Inglis and 20 by Alex Carey in the middle-order but the late innings boost came from number 7 Oliver Peake as the 20-year-old smashed an unbeaten 41 off just 18 balls, that included 3 sixes and two fours.
Masakadza was the best bowler on show for the hosts with figures of 2-51 in nine overs while seamer Brad Evans took three scalps but was expensive, conceding 86 runs nine overs.
Zimbabwe were always up against it as they set about a record run-chase with opening pair Brian Bennett and Ben Curran putting 43 inside 12 overs before the former was dismissed by spinner Matt Renshaw for 23.
Renshaw then struck a double blow with the wicket of Curran for 30 as Zimbabwe slipped to 60-2, with the middle-order then making solid but not good enough contributions.
Innocent Kaia (34), Brendan Taylor (39) and Craig Ervine (38) all got good starts hut failed to capitalise while skipper Raza struck five fours for a 49-ball 45.
Zimbabwe were constantly pegged back from gaining any momentum in the innings as Australia took wickets at crucial stages with seamer Josh Hazlewood 2-48 after getting through nine overs.
The spin trio of Connolly, Renshaw and Adam Zampa also took two scalps apiece as the home side were eventually bowled out for 272 in 48.3 overs as the Aussies took the series trophy with a game still to play on Sunday.
Glenn Maxwell has called time on his international career after not being included Australia's squad for the five-match T20I series at home against England that starts later this month.
Australia head coach Andrew McDonald admits Marnus Labuschagne "hasn't taken his opportunity" to cement his place in the Test team in the series in South Africa.
The Proteas blew Australia's batting order away on the fifth day of the deciding Test at Newlands, the visitors crumbling to 111 all out as the hosts wrapped up a 176-run victory and a 2-1 series win.
Steve Smith is expected to recover in time for Australia's opening Test against New Zealand in December after medical examinations ruled out significant damage to his neck.
