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The former Hartlepool and Wrexham keeper, 34, links up again with Town boss Richie Barker, who was manager at Bury where Williams was goalkeeping coach.
Barker told the club's official website: "Taff is a great addition to our management team.
"He worked with the Wales youth squad so he's got good knowledge of top youth football and of younger players around the country.
"And he knows how I want to work, the way I want to play and the sessions I put on. He is going to be a very valuable and important member of what I believe is an excellent backroom team."
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The Sussex club have also added former Brighton manager Martin Hinshelwood to their scouting team.
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