Tommy Smith, nicknamed the 'Anfield Iron' by supporters, has died aged 74, Liverpool have confirmed.
Smith, a former captain of the club, won four league titles during his 18 years with the Reds, for whom he made 638 appearances.
He was a key part of the side when Bill Shankly led Liverpool to their first FA Cup triumph in 1965 and 12 years later was on the scoresheet as they won their maiden European Cup by beating Borussia Monchengladbach.
"Tommy is survived by [daughter] Janette, son Darren and four grandchildren, Matthew, William, Jessica and Imogen," Liverpool said in a statement.
"The thoughts of everyone at Liverpool Football Club are with Tommy's family and many friends."
Smith, a fearsome defender, scored 48 goals and won nine major trophies with Liverpool.
He had two stints in the United States, with Tampa Bay Rowdies and Los Angeles Aztecs, and retired in 1979 after a spell with Swansea City.