By far the series' best bowler, Starc (77 runs off 141 balls) helped Australia finish their first dig in the second Test all out for a formidable 511.
That left England 177 runs shy of the hosts as they prepared to bat in the twilight but early breakthrough wickets weren't as forthcoming for Australia as previously in the series.
England (0-45) went to tea 132 runs behind Australia after openers Zak Crawley (26 not out) and Ben Duckett (13no) made a positive start.
At the crease, Starc had to navigate the second new ball as well as the loss of dangerous batting partner Alex Carey (63) en route to his highest score since 2016.
When Carey nicked off, Australia's innings appeared likely to peter out as they held a solid, though certainly not watertight, 82-run lead.
But by the time No.9 Starc holed out to Ben Stokes at mid-off, Australia had beefed that advantage up 75 more runs.
They'd also slowed the pace of the game down so as to ensure England would need to face the day-night masters bowling with a new pink ball in fading light.
Unless they can turn things around dramatically at the Gabba, Stokes' men will be left to defy history.
No England side has recovered from 2-0 down to win a five-match Ashes series.
Starc had raised his bat for a 12th Test half-century just after tea and then put his foot on the accelerator with back-to-back fours off Gus Atkinson (1-114).
When he lofted Atkinson past mid-on for another boundary, Starc usurped Jake Weatherald (72) to become Australia's unlikely top-scorer for the innings.
No man in Test history has scored more runs at No.9 than Starc, who passed former Ashes rival Stuart Broad during Saturday's second session.
Earlier in the game, he had taken six wickets and dethroned Pakistan's Wasim Akram as the most prolific left-arm pace-bowler in Test history.
Just when his Test high-score of 99 appeared in danger, Starc sent a short Brydon Carse (4-152) delivery to Stokes and left the pitch to a standing ovation.
Brendan Doggett (13) moved the impressive total past 500 with a four off Will Jacks.
Doggett's 13 is the highest lowest score in a completed Australian Test innings, but the No.11 was caught behind off Jacks to bring the innings to a close just after 6pm local time.
Earlier, Carey had flaunted his cover drive en route to a 14th Test half-century and appeared the man to build a game-defining lead for Australia before tea.
Instead, the wicketkeeper swatted at a Atkinson delivery wide of off stump, leaving Starc to do the dirty work.
Michael Neser (16) missed out on the lower-order runs that appeared on the table after he controversially replaced veteran spinner Nathan Lyon in the XI.
The paceman, who has made five first-class hundreds, was caught behind off an outswinger from workhorse Stokes (3-113).
England risk losing WTC points for their slow over rate, trailing by two at the change of innings.
Australia fell eight behind in their first innings with the ball but avoided punishment by bowling England out within 80 overs. Australia, though, were all out in 117.3.
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