Chew played drug kingpin "Proposition Joe" Stewart on the critically acclaimed crime series for its entire five-year run.
Chew's sister, Clarice, told The Baltimore Sun her brother died in his sleep Thursday. Funeral services will be held Jan.24.
David Simon, who created "The Wire," told The Hollywood Reporter Chew's performances included a series of consistently top-notch gems among "an embarrassment of riches."
"Robert's depiction of Proposition Joe was so fixed and complete -- from the very earliest scenes -- that the writers took for granted that anything we sent him would be finely executed," said Simon.
Chew also carved out an accomplished career as an acting coach in the Baltimore area. The Morgan State University graduate landed guest roles on "The Wire" for 22 of students, The Reporter said.