The townsmen of Galaxidi, where Vassiliou was born, collected money to send him to Athens in 1921, to study at the Athens School of Fine Arts under teachers Alexandros Kaloudis and Nikolaos Lytras.
Spyros Vassiliou became recognized as a painter of the transformation of the modern urban environment, depicting with an unwavering eye the sprawl of urban development that surrounded his home in Athens, under the walls of the Parthenon.