However, it wasnt all plain sailing. Mills himself wasn't too impressed by Tom's scruffiness, and record companies were finding his style and delivery to be too abrasive and raw.
Tom's vocals were considered to be too raucous, and he moved like Elvis. Not things that were expected of a Valleys boy in the early 60s!
Fortunately, Decca rekindled their early interest, and Jones recorded his first single, Chills And Fever, for them in late 1964.
The single didn't chart, but the follow-up, It's Not Unusual, was an instant smash hit. Its orchestrated arrangement coupled with Jones energetic delivery proved infectious, and the song reached number one in the UK and the top 10 in America. And so a star was born.
A string of hits followed, including Once Upon A Time, With These Hands and Burt Bacharach's classic What's New Pussycat.
In 1965 Tom sang the theme tune to the James Bond film Thunderball, which starred Sean Connery. He also met Elvis that year, starting a friendship that would endure until Presley's death in 1977.
In 1966, Tom released his most successful single ever: Green, Green Grass Of Home was to become Tom's second chart topper. He first heard the song on a Jerry Lee Lewis album, Country Songs For City Folks, but the song was interpreted by many to refer to Jones' native Wales.
The following year, 1967, Tom performed for the first time in Las Vegas, at The Flamingo. In future years he would return time and time again. Indeed, Tom's time in Las Vegas saw him elevated to superstar status in America, a position he enjoys to this day.
One of Tom's best-loved singles was released in 1968. Delilah was a dark tale of murder and infidelity, but people were entranced by the melody and Jones' unforgettable delivery. It became a big hit.