The young Princess Alexandra, daughter of King Christian of Denmark, came to England to marry the later Edward VII in 1863. Alexandra Road was built by the Eyre Estate.

A notable resident of Alexandra Road was Lily Langtry (1853–1929), music hall singer and, with little irony at the time, the mistress of the husband (Edward VII) of the woman that the road was named after.

Langtry’s house in Alexandra Road had to be demolished to make way for the 1970s Alexandra Road development and she is remembered in the name of Langtry Walk.

The story of Alexandra Road is a story of ’two halves’. There is a remaining section which has continued in existence since the 1860s.

Prior to the creation of the London Borough of Camden, the Eyre Estate had owned Alexandra Road and were developing plans for rebuilding the street in the early 1960s. The Eyre Estate had to abandon their first plan for a middle-class scheme of a high density mixed development, to accommodate their tenants on protected rents. Hampstead Metropolitan Borough had also become alarmed at proposals for tower blocks and recommended their rejection.

In 1965 the new London Borough of Camden bought the 13.5 acre site and their own architects department began a new design in 1968. The new estate, which involved the demolition of the western section of Alexandra Road was designed by the architect Neave Brown. Construction began in 1973.

A contemporary review commented that "the arrangement is similar to that of Regency or Victorian London and the scale approximates with the nearby Belsize Park.’ Brown added that he was inspired by London squares, Georgian Bath, Bristol and Leamington Spa. Referring to the tower blocks that could have been built, Brown noted "The cautionary tale stands 20-storeys high across Abbey Road, and the form of Alexandra Road can regrettably be read as a frame for, and parterre to, the rejected model."