The South African will continue in his role as Derbyshire head of cricket and work with Pakistan outside the county season.
Arthur wil be part of the Pakistan coaching staff for the 2023 Cricket World Cup in India, a tour of Australia, a home series against West Indies and the Asia Cup contests with India.
During his tenure as Pakistan head coach from 2016 to 2019, the 54-year-old mastermind an ICC Champions Trophy success six years ago, while he also took the Test and T20I sides to the top of the rankings.
The former Australia and South Africa coach said: "I am absolutely thrilled to be rejoining the Pakistan cricket team and look forward to working with the group.
"Since moving on, I have kept a track of the players and their collective performances.
"This is a talented bunch with the potential to be number one across all formats and my endeavour is to put in place strategies and create an environment that can contribute in further enhancing their performances so that we can extract the best out of them."
The Pakistan Cricket Board had revealed in January that they held talks with Arthur with a view to making him Saqlain Mushtaq's successor as head coach, but could not reach an agreement.
The Pakistan Cricket Board (PCB) held talks with Arthur with a view to appointing him as successor to Saqlain Mushtaq, whose contract expires at the end of next month.
Arthur only signed a new three-year deal to extend his tenure as Derbyshire head of cricket last month and the vastly experienced 53-year-old will not be returning for another spell with Pakistan.
A PCB statement released on Tuesday said: "The Pakistan Cricket Board today confirmed it has been in talks with former national team head coach Mickey Arthur with a view to appointing him as the head coach to guide the side through to the ACC Asia Cup, ICC Men's Cricket World Cup 2023, ICC Men's T20 World Cup 2024 and the ICC Champions Trophy 2025.
"However, owing to his long-term contract with Derbyshire, we have also discussed a proposal to act as a consultant to the PCB on a time-sharing basis with Derbyshire.
"Unfortunately, however, this option is proving difficult to materialise for various reasons on both sides.
"Under the circumstances, the PCB will continue its search for the right person to fit the slot of the national team head coach and some top names are already under consideration."
Arthur masterminded Pakistan's 2017 Champions Trophy triumph in England and also took the team to the top of the Test and Twenty20 International rankings before leaving the role in 2019.