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In his third knock in green and gold since returning from a year-long suspension, the former Australia captain breezed to 91 from 108 balls against a below-strength New Zealand XI at Allan Border Field on Friday.
Australia were 5-248 after 44 overs - in pursuit of the Black Caps' 9-286 - when bad light stopped play, the hosts claiming a five-wicket win under the Duckworth Lewis method to win the unofficial series 2-1.
Batting at No.3, Smith drove superbly and was rarely troubled in his last hit out on Australian soil before the squad left for England - via Gallipoli - on Friday night.
That innings followed an unbeaten 89 on Wednesday as Smith, who had surgery on his elbow in January, finds his groove ahead of their World Cup opener against Afghanistan on June 1.
There were anxious moments though, Smith dropping his bat when his bandaged arm jarred as his blade stuck in the turf when completing his 64th run.
Smith flexed the joint in the overs that followed and received some brief physiotherapy treatment at the next drinks break before batting on without discomfort to flirt with a triple figure score.
"His timing, his class was back again," captain Aaron Finch said earlier in the day of Smith's innings on Wednesday.
"It was like he hadn't left.
"His driving down the ground on a difficult wicket ... to time them was so impressive.
"Just the way he was able to go through the batting gears was very impressive."
Glenn Maxwell (70 off 48) made his second consecutive half century, reaching 50 off just 37 balls before reverse-sweeping a six into the small crowd at cover, as he dominated a 104-run partnership with Smith.
David Warner followed his Wednesday duck with just two at the top of the order while Usman Khawaja (23) and Shaun Marsh (32) made starts.
Earlier Pat Cummins (4-32 from eight overs) was the pick of Australia's bowlers, while the visitors took a liking to Adam Zampa's leg-spin as he finished with 2-76 from nine overs.
Mitchell Starc got through eight overs, taking 1-35, in his second game back from a pectoral injury.
Will Young was again New Zealand batting star, his 110 off 108 balls following 130 on Wednesday and 60 on Monday.
The 26-year-old isn't part of the Black Caps' Cup campaign though, booked for imminent shoulder surgery and set to miss between up to nine months of cricket.