Entering the legal profession, Samuels was called to the bar at Inner Temple in 1948. The following year he emigrated to Australia and worked as a clerk for Dawson Waldron Edwards and Nicholls (now Ashurst Australia). Called to the New South Wales bar in 1952, Samuels gained a reputation as being a "persuasive advocate and destructive cross-examiner". He married Jacqueline Kott in 1957 and had two daughters named Deborah and Selina. Between 1964 and 1970, he was the Challis Lecturer of Law in Pleading at the University of Sydney. In 1964, he was appointed Queen's Counsel for New South Wales and later for Victoria in 1965. In 1971, Samuels was elected as the President of the New South Wales Bar Association, in which capacity he served until 1972.