Smith's no-nonsense performances at the heart of Liverpool's defence saw him nicknamed the 'Anfield Iron' during his 18-year spell on Merseyside.
Making 638 appearances for the Reds between 1960 and 1978, Smith won a host of medals as the club rose to prominence both domestically and in Europe.
Under the management of the great Bill Shankly, Smith helped Liverpool dominate for two decades.
Reflecting his tough style of play, Shankly once said of one of his favourite players: "Tommy Smith wasn't born, he was quarried".
Smith, who captained the club for three years, was one of the most influential members of the Liverpool team that won the FA Cup for the first time in 1965.
Twelve years later, with Bob Paisley at the helm, he would head a crucial goal as Liverpool won their maiden European Cup by defeating Borussia Moenchengladbach in the 1977 final in Rome.
In total, Smith won the English title four times, the FA Cup twice, the European Cup once and the UEFA Cup twice.
Speaking to Liverpool's official website, Smith's daughter Janette Simpson said: "Dad died very peacefully in his sleep shortly after 4.30pm today.
"I was on my way to see him when he passed a couple of minutes before I arrived.
"He had been growing increasingly frail and suffering from a variety of ailments over the last three months especially. We are obviously all devastated."
Smith's former Liverpool team-mate Phil Thompson told Sky Sports that his fellow defender was an 'icon'.
"I loved him from the Kop, because of his passion, commitment and never-say-die attitude," he said.
"To go on and play with him, rub shoulders with him, go into battles with him, he was iconic. He wanted and desired the points every week."
Former Liverpool player and manager Kenny Dalglish added: "He was a great advert for Liverpool Football Club, the way he conducted himself. His memories will be there forever."