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Smith and wicketkeeper Brad Haddin, however, put on 124 for the sixth wicket with circumspect and, occasionally, aggressive innings that contrasted sharply with the cavalier efforts of their team mates and Australia reached the close on 326 for six.
They were separated when Haddin, who has scored half centuries in all four innings in the series, spooned the ball to James Anderson at midwicket off the bowling of Ben Stokes for 55 an hour before stumps.
Smith reached his second test century, however, and will resume on Saturday on 103 not out with Mitchell Johnson, unbeaten on 39.
“Yeah it was nice,” Smith told reporters. “Obviously under a bit of pressure there losing a few wickets in the middle but hopefully we’re in a decent position.
“If we start well tomorrow, we can post a really good score.”
England were left ruing a missed opportunity to take control of the test and bowling coach David Saker was disappointed his paceman had let Australia off the hook by not bowling a consistent length.
“No doubt we let it slip,” he said. “It’s probably not the first time this series as well we’ve had them on the ropes to a degree and we haven’t finished the job.”
After losing the toss for a third successive match and the chance to bat on what looked like an excellent surface, the tourists initially responded to their do-or-die situation with their sharpest display of the series to date.
Australia’s batsmen looked intent on piling on the runs as quickly as possible - they were scoring at five an over at one stage - but also contributed to their own demise with rash strokes.
David Warner’s attempted cut only to be caught at point for 60 would contend for the softest dismissal of the day but Bailey (seven) also came close to claiming the honours with a hook that saw him hole out on the boundary.
Captain Michael Clarke (24) will also be disappointed with the shot that led to his departure just before lunch, a wicket which followed the run out of opener Chris Rogers (11) and dismissal of Shane Watson (18) in the first hour.
England spinner Graeme Swann, under pressure after disappointing displays in the Brisbane and Adelaide defeats, made a significant contribution by catching Watson well in the slips before accounting for dangermen Clarke and Warner with his bowling.
Seamer Stuart Broad took the wickets of Watson and Bailey and England, if not in charge, certainly had the upper hand at a ground where they have not won since 1978.
Smith had already signalled his intent with a big six to get off the mark, however, and when he was joined by Haddin, Australia’s rearguard was in place.
While Smith played his scoring shots almost exclusively to the on side, Haddin favoured off but they both brought up their half centuries from 76 balls with five fours and two sixes.
With the temperatures out in the middle now exceeding 40 degrees Celsius, the pair forced England to labour long into the extended final session under the blazing Perth sunshine.