He soon began to patronise the arts around 1829, both in Britain (where his protégés included Edward Calvert and George Frederic Watts, who became his friends) and in Greece (where he followed his father as a patron of the University of Athens).

Afterwards they moved to Tulse Hill (1838–1864) and finally to 1 Holland Park (1864 onwards), during which time began to gather an artistic salon at his home.

His son Alexander introduced him in 1860 to artists whom he had met in Paris, such as James Abbott McNeill Whistler, Edward Poynter, Thomas Armstrong, and George du Maurier; later Dante Gabriel Rossetti and Edward Burne-Jones also joined Ionides's circle.

He commissioned the designers Philip Webb and Thomas Jeckyll to redecorate 1 Holland Park.

In 1875, he finally moved to a house called "Windycroft" in Hastings, leaving Alexander to complete the Aesthetic redecoration at 1 Holland Park by commissioning William Morris and Walter Crane).