Williams' son said his father died Thursday after an illness at St. Mary Mercy Hospital in Livonia, a Detroit suburb.
Williams played for Detroit from 1960-65, after a year with the Los Angeles Rams. He spent his final two NFL seasons in Atlanta.
He played on the Lions' defensive line that included Alex Karras, Roger Brown and Darris McCord.
Williams was a star player at Michigan State before heading to the NFL. He grew up in Dansville, outside Lansing.
A funeral will be held Sunday. Williams is survived by his wife, Lois, two sons and two sisters.