Williams was part of the coaching staff of the Wolves under-23 side which was crowned Premier League 2 Division 2 champions this season.
He will now join Mark Robins’ coaching staff at the Sky Blues as he pursues his dream of coaching at first-team level.
Wolves’ head of academy, Scott Sellars, said: “Aled has played a huge role in the under-23s’ success this season.
“We thank him greatly for his service to Wolves and wish him all the best as he takes an opportunity to coach at first-team level.”
Speaking to Wolves.co.uk, Williams said: "I have spent four fantastic years at Wolves and have loved every single moment of it.
"I have had the pleasure of working with some excellent goalkeepers, players and outstanding staff at the club and Academy.
"I would like to thank Kevin Thelwell and Scott Sellars, and everyone at the Academy for their support given on and off the field in my personal development and that of my role here at Wolves," he continued.
"I would also like to pay a huge thank you to Rob Edwards, Sean Parrish and all the under-23 staff and players. The work rate and togetherness of this group was exceptional and I think the season just gone exhibits this."
Everyone at Wolves would like to wish Aled all the best for the future.