Previously elections had taken place in the Municipal Borough of Harrow.
A total of 168 candidates stood in the election for the 56 seats being contested across 15 wards.
These included a full slate from the Conservative and Labour parties, while the Liberals stood 50 candidates.
The Council was elected in 1964 as a "shadow authority" but did not start operations until 1 April 1965.
The results saw the Conservatives gain the new council with a majority of 16 after winning 36 of the 56 seats.