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Jackett has been out of work since leaving League One Portsmouth in March and has put pen to paper on a one-year rolling contract with Orient.
The 59-year-old brings with him a wealth of experience and is something of a coup for the League Two side.
Jackett has previously worked with Watford, Swansea, Millwall, Wolves and Rotherham, enjoying plenty of success.
He won League One with Wolves and also enjoyed promotions with Swansea and Millwall too.
After parting company with Pompey in March, Jackett has been eyeing his return to football, and saw Leyton Orient as the club perfectly matching his own ambitions.
“I see Leyton Orient as a club full of potential. That’s the attraction. My own personal ambition is to take us to the next level,” he said.
“We really want to hit the ground running, unite the club and be successful in the coming season. Squad planning is vital. The summer is such an important time.”