The best-known of Grey Street's great homes was Eildon Mansion, built in 1877 by the wealthy pastoralist John Lang Currie.
Another well-known landmark on the street in the 19th century was the St Kilda Coffee Palace, now a backpackers' hostel.
During the 20th century the social status of St Kilda declined and the wealthy moved away from Grey Street.
The Church operates a large welfare centre, the Sacred Heart Mission, near the corner of Grey and Robe Streets, providing meals and sleeping accommodation to the homeless and needy.
The Salvation Army operates the St Kilda Crisis Centre on Grey Street, offering services including a needle exchange facility for drug users.