The Eyre family were local landowners and became keen to promote building. In 1794 a plan was drawn up on the model of Bath, with a crescent, circus and a square. The plan was never executed but from 1802 development on the Eyre estate was directed by John Shaw, a young architect inspired by the town-planning ideals of the late 18th century. In 1803-4 he exhibited views of a projected circus and in 1807 building began on the Marylebone portion.

In 1819 Col. Eyre began the first of several attempts to promote the construction of a public road through his estate, ultimately successful in the Finchley Road Act of 1826. Finchley New Road and Avenue Road, the southern part of which existed by 1824, went northward into the Hampstead portion of Eyre’s land and were built by 1829. The Swiss Cottage tavern was built at the apex of the two roads by 1841.

College Crescent was then laid out in the 1840s, and by 1852 the first thirteen houses had been built there. These houses were stuccoed terraces with iron balconies built by W. Wartnaby.

More buildings included the school for the blind, built in 1848 at the southern junction of College Crescent and Avenue Road and enlarged in 1864, 1878, and 1912; of brick with stone dressings, it had an Italianate central block with two wings.

The North Star pub opened in 1850 and, enclosed by the curve of College Crescent, the New College of Independent Dissenters, for training ministers, was opened in 1851 in a building designed in an early Tudor style by J. T. Emmett. He also designed the college’s Gothic chapel, opened soon afterwards to the south, at the junction of Avenue Road and Adelaide Road.

Immediately south of the blind school a large house, Sunnyside (later St. Columba’s hospital), with a Greek Doric porch, was built by 1862.

Samuel Palmer, of the biscuit firm, lived at no. 40 College Crescent, a large house called Northcourt built in 1881.

New College and much of College Crescent were pulled down in 1934 and replaced by Northways, two concrete blocks of flats and shops by London & City Real Estate.

Redevelopment of the site previously occupied by the school for the blind, St. Columba’s hospital, and the New College Chapel, was considered in 1957. A scheme for a civic centre was published in 1959 by the architect, Basil Spence, and part of it, the library and the adjoining swimming baths, was opened in 1964.

In 1962 Hampstead theatre opened on a site north of the library that had been intended for civic buildings.

Originally the street has three names along its length. From the North Star it was ’College Villas Road’. The following section was ’College Terrace’. Only the final section near to the Blind School was it ’College Crescent’.