Smith and David Warner returned to Australian colors earlier this month after serving their one-year bans for involvement in a ball-tampering scandal in Cape Town last year.
The duo took part in three warm-up matches at home to a second string New Zealand side, but Wednesday's unofficial warm up contest was their first outing in England since completing their bans.
The unofficial match saw Smith lead the way once again as he guided Australia to a modest target of 230 in a seven-wicket win against West Indies.
But there was a slight concern for the Aussies when top-order batsman Usman Khawaja was struck on the jaw by a sharp Andre Russell bouncer and retired hurt following on-field treatment.
He was later sent to hospital for a precautionary X-ray.
Warner only made just 12 when he was undone by a brutal bouncer from Oshane Thomas that he could only manage to fend it to the wicket-keeper.
Earlier, West Indies were bowled out for 229 with Evin Lewis and Carlos Brathwaite scoring half-centuries.