Harris's second first-class ton of the season helped Victoria reach 6-282 at the end of a tough day one for Queensland at the MCG.
As Australia's top order struggled in India, Harris played a chanceless innings before being dismissed for 100 just two balls after reaching the milestone.
The opener found the boundary rope 12 times and also struck two sixes in posting his 24th first-class ton from 146 balls.
Harris played the last of his 14 Tests in January last year against England, but was included in Australia's squad during the recent series against the West Indies and South Africa.
He enjoyed strong support from breakthrough star Ashley Chandrasinghe, with the pair adding 119 for the second wicket.
The rookie No.3 looked on track for his second Shield century in five outings before a patient knock of 67 from 186 balls was ended.
Chandrasinghe played across the line to be trapped lbw by left-arm spinner Matthew Kuhnemann (2-55).
Earlier Kuhnemann induced a top edge from a Harris pull shot as the opener offered a simple catch to Xavier Bartlett at square leg.
Bartlett had already held a high catch as Travis Dean skied a pull shot off Liam Guthrie to fall for six.
It was just the fourth ball for Guthrie in Queensland colours since a move from his home state of Western Australia.
But it was to prove one of the few bright moments for Queensland after skipper Jimmy Peirson elected to send the home side in to bat after winning the toss.
Matt Short and 20-year-old rookie Campbell Kellaway added 48 until the latter edged Bartlett into the slips to fall for 41.
Queensland enjoyed late success with the new ball with three wickets falling in the final hour.
After Kellaway's dismissal, Short was bowled by Mark Steketee (2-55) for 48, while the paceman also knocked over Mitch Perry for a duck.
Acting captain Will Sutherland ended the day with an unbeaten run-a-ball 26 with Sam Harper also at the crease (four not out).
Sutherland skippered Victoria for the first time with regular captain Peter Handscomb on representative duty in India along with teammates Scott Boland and Todd Murphy.
With six rounds completed before Christmas, Victoria will likely leapfrog second-placed Queensland with a win in the four-day encounter.
