Just 11 days out from the first Test in Perth, Starc worked his way through Victoria's top order on Monday to finish the opening day of the match with 4-91.
Peter Handscomb was Victoria's best, hitting his second century of the summer before being bowled by Nathan Lyon for 104 late in the day.
Lyon (2-65) also had Marcus Harris caught at bat-pad early, while Josh Hazlewood (0-54) got through his 18 overs unscathed and bowled with good rhythm.
But it was Starc who looked the most dangerous, playing his first Shield match of the summer ahead of an Ashes series where he will again be Australia's point of difference.
Bowling with genuine speed, Starc was on song early and had Harry Dixon lbw for 20 with one his trademark yorkers that tailed back in at the left-hander.
The left-armer's battle with Campbell Kellaway was the highlight of the day, in a high-quality first hour of the second session.
Starc struck the Victorian opener on the fingers once, while another ball ballooned off the gloves and just over Steve Smith at second slip.
Kellaway did well to progress to 51, but Starc eventually had his man when the left-hander gloved a ball down the leg side to wicketkeeper Josh Philippe.
Oliver Peake came and went quickly, superbly caught by Kurtis Patterson when he crunched his third ball from Starc to gully.
And while there was a hint of the BazBall approach from Victoria and Sam Harper (54) after tea, Starc withstood the onslaught and prevailed.
Harper hooked Starc for one six deep into the Brewongle Stand and pulled him for another towards the Members Pavillion.
But after the Victorian took 22 runs from the first five balls of a Starc over to bring up his half-century, the left-armer had him caught on the mid-wicket boundary.
Starc bowled 18 overs in total, playing his first red ball match since claiming 6-9 in the fourth innings against West Indies in Jamaica in July.
Handscomb showed a calm head throughout.
He made the most of a life after being dropped on nought when he edged Hazlewood to Jack Edwards at slip.
After that, the Victorian was able to accumulate runs, regularly scoring behind the wicket and producing a fine cover-driven four off Sean Abbott to get in the groove.
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