The 26-year-old joins on a two-year deal after a productive 2022-23 campaign at Crewe Alexandra, having netted 16 goals and added five assists.
Agyei was named player of the season for the Railwaymen and hopes to make an impression on supporters in E10 as well.
“I’m the one that likes to dribble with the ball, beat players and create chances,” he told the club website.
“The fans are in for someone that will work hard, but also be a livewire on the pitch.
“I like the way Orient played and the attackers had a lot of freedom, so coming here felt like a great fit.”
London-born Agyei began his career at AFC Wimbledon and, after joining Burnley for an undisclosed free, moved to League One Coventry on loan, netting on his debut at Bradford.
He returned to the Clarets and made his Premier League debut as a substitute against Liverpool at Anfield, then had further loan spells at Walsall and Blackpool.
He turned down a contract offer to stay at Burnley and joined Oxford in 2019, but moved back to the north west and Crewe two seasons later for an undisclosed fee.
And head coach Richie Wellens was impressed by what he saw during the three matches between Crewe and O’s last season.
“Of all of the opposition last year he was probably the standout player, and with a really good return in terms of 16 goals at Crewe,” said Wellens.
“He scores all different types of goals, using pace, power, a good left foot, and scores headers.”
“At 26 years old he’s at a good age, and we think he can kick on.”
Agyei is the second new signing for O’s this summer, with Max Sanders having joined on a two-year deal last week.
Home-grown defender Dan Happe, 24, has also signed an extension to his contract until the end of the 2023-24 season, with an option for a further year.
The former Academy youngster has made 185 appearances for O’s so far, scoring three goals, but saw his season cut short by a knee injury.
He said: “I’d say last season was my best footballing season for the club. I was unfortunate to pick up another injury, but I’m happy to have signed this extension now and to be staying with the club.
“It was nice to get some minutes at the end of the season, I want to say thanks to the gaffer for that one. I’m back fully fit now and I want to prove that I can play well and stay fully fit for the whole season.
“I feel like people could doubt me now because of my injuries, but I want to prove that isn’t the case.
“The gaffer plays a big part in how I play and how I perform, the things he wants to do suits me down to the ground. The players in the changing rooms and on the pitch really help me.
“Football moves on and people have moved on, but we’ve got a core group of people who were here last year and there’s no doubt for me that we’ll crack on again and do what we do best.”
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