Cipriani's last appearance at Twickenham was with England in the autumn of 2008, after which he was cast into the international wilderness by Martin Johnson.
The Barbarians were overwhelmed by Australia, who ran in eight tries, leaving Cipriani with little chance to shine at fly-half.
But the 24-year-old impressed the Barbarians' World Cup-winning coach Graham Henry during the week and reiterated his desire to break back into the England fold.
"I loved it, running out at Twickenham, hearing that roar. It is probably the best stadium in the world in terms of rugby and I have massive ambitions to be back here playing," Cipriani said.
Australia scored 42 second-half points with Digby Ioane, Lachie Turner and James Horwill all touching down twice.
There were tries for Rob Horne and Radike Samo while James O'Connor, Cipriani's new Melbourne Rebels club-mate, kicked 20 points.
The Barbarians' defence was embarrassing but they did give the 51,212 crowd a late cheer with a late consolation try for England rugby league international Sam Tomkins.
The Wigan full-back had never played a game of rugby union before in his life but acquitted himself well - despite starting the week not understanding any of the positions.
"When I came in on Tuesday I was so raw I didn't even know what the numbers for each position were," said Tomkins, whose brother Joel has signed for Saracens.
"The boys were saying 'we'll play this off the 12 or the 10' and I didn't even know where those blokes were so that was a bit of a challenge.
"There are so many differences between league and union. I understand it a little bit more now.
"Where I am from people don't know what rugby union is and I am glad I have had the chance to play but I am still a rugby league player.
"The try was a good way to finish it off but we didn't manage to get much going."
On the same day his brother joined Saracens, Tomkins announced he had agreed a new deal with Wigan but there is already talk of a cross-code switch in three years.
Graham Henry believes he would be a valuable acquisition.
"There's no doubt that Sam's a talented footballer who will be a big success in either rugby code," Henry said.
"He had never played union before - he didn't know what a ruck was or what a maul was. He has got good balance, he's quick and he's got a good head."
Australia coach Robbie Deans described his side's victory as "ideal", one week before the Wallabies tackle Wales in a re-match of the World Cup bronze-medal decider.
The Wallabies won that encounter in Auckland and Deans expects to come across a fired-up Welsh side at the Millennium Stadium.
"That is going to be a tough assignment so it was good to have a hit-out," he said.
"We expect a lot. We have been reading it, we have been hearing it. They, like us, weren't happy with the way they exited the World Cup.
"Sam (Warburton) was very frustrated not to be involved at the death (after being sent off in the semi-final) and you have got Shane Williams' last fixture. There will be a bit of emotion there."
Australia captain David Pocock is looking forward to his clash with Warburton.
"From our experience that disappointment is definitely there. You want to make amends for it and he will be no different - probably more so," said Pocock.
"I am looking forward to the battle of the breakdown."
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