Best attended the Tacarigua Anglican School and Queen's Royal College, in Port of Spain. He won an island scholarship and graduated from the University of Cambridge and Oxford University. In 1957 Best joined the Faculty of the University of the West Indies in Mona, Jamaica as a Research Fellow.
He remained as a Professor in Economics until 1976, when he resigned to work full-time at Tapia House, a political, social and economic organisation. Tapia House was unsuccessful in gaining seats in the 1976 elections, but some the party's members helped form the National Alliance for Reconstruction, which won the 1986 General Elections.
He was Leader of the Opposition in the Senate from 1974-1975 and 1981-1983. He was also the founder of the Trinidad and Tobago Institute of the West Indies (known since 2007 as the Lloyd Best Institute of the West Indies).
Even though he was in failing health, two weeks before his death Best was hard at work with his colleague and fellow Tapia house member, Eric St Cyr completing his newest work titled Economic Policy and Management Choices: A Contemporary Economic History of Trinidad and Tobago, 1950-2005.
He died at his home, aged 73, from prostate cancer and diabetes. He was twice married, first (1958-2006) to Christiane Best with whom he had 4 children and is survived by his second wife, journalist Sunity Maharaj with whom he had two daughters.