In 1846–1849, he served in Ireland during the Great Famine, as temporary inspector with special duties under the Poor Law Commissioners.

[9] In 1850, he retired on half pay as a lieutenant-colonel and joined the Metropolitan Police as its second inspecting superintendent, effectively functioning as deputy to the two Joint Commissioners, Sir Richard Mayne and Captain William Hay (who had been his predecessor as inspecting superintendent).

He was appointed Companion of the Order of the Bath (CB) for his services in policing the Great Exhibition in 1851 and in 1855 was selected to attend Queen Victoria in Paris.

After Mayne's death on 26 December 1868, Labalmondière acted as Commissioner until the appointment of Colonel Edmund Henderson three months later.

He continued to serve Henderson and his successor, Sir Charles Warren, as Assistant Commissioner until his retirement in 1888.