The highest successful chase in a Gabba Test was in 1951 when Australia finished 236 for seven, but there have been big scores in recent years.
It means all outcomes are possible entering the final day of an epic series, which is tied at 1-1.
Indian openers Rohit Sharma and Shubman Gill then faced just 11 balls, reaching four without loss, before light rain ended play.
The call for Steve Smith's reappointment as the Australia captain in Test cricket is gathering momentum with the legendary Ian Healy advocating his return to the top job in the next "12 to 18 months". The hosts now have a lead of 54 runs.
Sundar who also took three wickets in the first innings added 123 runs for the seventh wicket with Shardul Thakur (67).
It was Thakur who made certain of his team-mate's five-for, taking the catch to remove last man Josh Hazlewood (9) and set up what promises to be an intriguing climax.
India's bowlers chipped away all day, with Siraj finishing the best of them with a haul of 5-73.
Smith said the match was well-poised, and typical of a series that as "ebbed and flowed" throughout. Holders India, however, need only a draw to retain the silverware after their breakthrough 2-1 win in the 2018/19 series in Australia.
'The game is in a nice place for us, ' Smith said.
Before the start of play on day four of the ongoing Gabba Test, Bumrah and Ashwin were seen practicing their skills.
The Brisbane pitch is showing a variable bounce as the cracks have opened a bit.
"Today a few balls shot up so tomorrow it's going to be case of hitting the right areas and letting the natural variation of a day five wicket do its work, and hopefully we can hang on to the chances". But replays clearly confirmed the dismissal.
Australia captain Tim Paine scored a quick 27 before he was caught behind attempting a hook off Thakur just before the tea interval.
The Australian openers added 68 runs off 19 overs when, with the score on 89, Harris fell for 38 when he tried to duck a Thakur short ball only for the ball to graze his glove on the way through to wicketkeeper Rishabh Pant.
Australia must force victory on the final day to regain the Border-Gavaskar Trophy, which will remain with India if the match - and series - ends in a draw.