It was a perfect response from Smith which may have the Barmy Army rethinking its strategy to get in his head.
He hit eight fours and three sixes — including two spectacular shots to clear the rope. One was an astonishing slap over point, prompting disbelief from commentator Mark Nicholas.
"Unbelievable from Steve Smith, how does he get it there?" Nicholas said. "That's an unbelievable stroke."
Later in his innings when he was upping the ante, Smith got inventive and ramped a ball over the wicketkeeper for another stunning maximum.
David Warner too copped some attention from the crowd when he walked out to bat but there was also some tepid applause for him. He was Australia's second top-scorer, hitting 43 off 55 balls with five fours as he opened the batting alongside captain Aaron Finch.
Warner and Usman Khawaja have shuffled around between opening and No. 3 in recent warm-up games and this time there was another ingredient added to the mix when Shaun Marsh was promoted to first drop. He was caught down the leg side for 30 and Khawaja came in at No. 5, reaching 31 before he was stumped.
Marcus Stoinis was filthy to be run out for 13 and while wickets fell regularly in the latter part of the innings Smith stood firm, before being controversially dismissed caught and bowled in the final over.
In reply, England chugged along as neither side was able to grab the ascendancy. Smith spilled a sitter at first slip to rob Jason Behrendorff of an early wicket but the left-arm quick bounced back to claim Jonny Bairstow for 12.
Jason Roy (21 from 37 balls) looked threatening but was unable to convert a start, picking out Nathan Lyon at cover off the bowling of Kane Richardson, leaving James Vince and Ben Stokes to build a partnership. Unfortunately for the hosts, Stokes lost a battle of wits with Lyon and was stumped for 20 when he charged down the wicket only to watch the ball spin past him and into the safe hands of Alex Carey behind the stumps. That left England at 3/100 in the 22nd over.
Enter Jos Buttler, who exploded with a scintillating cameo. The most damaging batsman in short-form cricket right now gave fans a taste of what they can expect at the World Cup as he cracked five fours and three sixes in rapid time. But shortly after raising his bat for a half century he chipped Nathan Coulter-Nile to mid-wicket, out for 52 from 31 deliveries.
Vince had lots of responsibility on his shoulders but guided Behrendorff straight to gully on 64 to give the paceman his second scalp. That saw Chris Woakes join Moeen Ali as England progressed to 5/220 after 38 overs.
Adam Zampa picked up his first wicket when Ali holed out to long on for 22 and Tom Curran fell soon after as England slumped to 7/250 but Woakes kept hopes of victory alive before he was run out for 40, leaving the hosts needing 23 from 16 balls.
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Liam Plunkett was joined in the middle by Adil Rashid, even though the leggie wasn't named to play and didn't bowl or field. He and Jofra Archer were allowed to bat in place of Liam Dawson and Mark Wood, who were injured earlier in the day.
Plunkett (19) picked out Glenn Maxwell in the deep on the first ball of the final over with England requiring 15 for victory and a run out secured Australia's win as the men in blue were all out for 285.