He then went to Trinity College, Cambridge and in 1909 was elected to the Isaac Newton studentship at the National Solar Physics Observatory.

In 1916 he enlisted in the Royal Engineers (meteorological section) and during the war years did important work related to atmospherical conditions at low levels in chemical warfare.

He continued his personal research and accepted Sir Napier Shaw's invitation to join him as part-time professor of meteorology at the Imperial College, London.

After the retirement of Sir Napier Shaw, Brunt became the first full-time professor of meteorology in Britain, holding the chair from 1934 to 1952.

[5] While he was working at Caerleon in 1915, he married Claudia Mary Elizabeth Roberts of Nant-y-glo, Monmouthshire, who had been a fellow student both at Abertillery and Aberystwyth.