The man known as "Nipper" has been overseeing the club's junior coaching since the move back to Altrincham.
But the 49-year-old former Trafford Metros player has accepted the offer to become coach Tony Hand's match-day assistant following the Scot's decision to carry on playing this season.
"I have been offered the chance before and did it for one night a couple of years ago but was not happy with it at the time," said Bayliss who takes over from David Graham.
"But now I think the time is right and I am always looking at ways to broaden my experience.
"I'm looking forward to working alongside Tony and forming a successful partnership.
"I have a lot of experience but not of working with professionals.
"I have always believed that team work is the key to success and, hopefully, I can help Tony forge a winning team."
Bayliss picked up the hockey bug as a teenager at Altrincham and was known for being a tenacious competitor.
Keen
He has been coaching for the past 20 years and is a keen student of the game, regularly attending coaching courses in Canada.
Meanwhile fans' favourite Brett Clouthier is looking forward to returning to action with the Phoenix.
"The support I've had from the fans in Manchester was a big factor in my re-signing, and in the way I play on the ice," he said.
"When I play and hear the fans chanting my name, it gives me that extra little push to make a hit, score a goal or win a fight.
"The fans in Manchester have been like a sixth player out there for me. I know they like the fighting and when they cheer for me as much as they do, I'm willing to drop someone to get them going even more."
Clouthier is also looking forward to meeting his new team-mates in a largely reshaped team.
"I don't know too much about the new guys Tony has brought in this year, I just know the guys that I played with last year," he admitted.
"I know Tony takes a lot of time researching and recruiting these guys, so I know they must be great players. I'm really excited to meet and play with all my new team-mates.
"Part of the fun will be getting to know them and helping them settle in.
"Our primary goal is to win and with a bunch of first year guys, to England, coming over to play, I'm sure that's exactly what they'll want to do too.
"It's only a couple of weeks now, I can't wait to get back, get training with the boys ready to put on a show for the fans in Manchester."
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