Bolton, who helped the Swans to the 2005 flag before retiring in 2010, has been appointed deputy general manager of AFL NSW/ACT, supporting general manager Harley.
A two-time All Australian, Bolton began his career in Canberra before going on to play 199games with the Brisbane Lions and the Swans.
"This is a fantastic opportunity for me to get back into the football environment and contribute to the community that gave me so much during my career," he said.
"I’m looking forward to sharing my experiences with the organisation during a dynamic and exciting time for the sport in this region."
Harley, who captained Geelong to two flags before rising through the ranks at AFL NSW/ACT, was pleased to have Bolton on board.
“Craig is a proven leader with values that firmly align with our working code and a desire to work in the AFL industry again,” he said.
“Once it was determined that Craig was interested in returning to the industry, I, with the support of the AFL executive in Melbourne, began to look at opportunities to have him in involved.
"We are extremely fortunate to be able to welcome a person of Craig’s talents and character into our team.”
Since his retirement, Bolton has been working as a consultant with a company specialising in human performance and training in Australia and the United States, before deciding to return to football.
James Dampney is a reporter for AFL.com.au. Follow him on Twitter: @AFL_JD