Jones was sacked by England last week after seven years in charge as he paid the price for the team's worst run of results during a calendar year since 2008.
England won only five of 12 Tests in 2022, a miserable streak that came after Jones led them to three Six Nations titles and the 2019 World Cup final.
The 62-year-old Australian is set for a quick return to the headquarters of English rugby union with Barbarians.
Jones previously coached the Barbarians in a 33-31 defeat by Fiji in 2019.
He will take on a world side coached by former All Blacks boss Steve Hansen on May 28.
"I am very much looking forward to returning to Twickenham Stadium - a venue I have so many fond memories of - as head coach of the Barbarians, and I'm more motivated than ever to put on a show," Jones said in a statement.
"Going up against Steve rekindles a great rivalry which first started in our days competing in Super Rugby and progressed into the international arena. It'll be a great challenge and one I'm sure we're both relishing."
