Dunford will take up a similar role at Plymouth Argyle.
He said: “My decision to leave Chesterfield FC is obviously tinged with sadness but the opportunity of working for Plymouth Argyle has a tremendous pull as I have previously worked there and still live in the city.
“I would like to thank everyone connected with the club, including supporters, for making me feel so welcome since I arrived in October last year. Come on you Spireites!”
Spireites’ director and company secretary Ashley Carson added: “I would like to thank Michael for the valuable contribution he has made during his time with us.
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“Michael has had to deal with a lot of internal re-structuring recently and has conducted this with the utmost professionalism.
“It is disappointing that we are losing Michael but I fully understand his reasons for wanting to join a club close to his home.
“I would like to wish him and his family all the very best for the future.”