Psarantonis comes from the mountainous village of Anogeia in Crete which during World War II was destroyed by the German occupying forces, when he was just two years old.

[1][2] He first played the lyre at the age of 13 and recorded his first single in 1964, titled "I Thought of Denying You" (Greek: Εσκέφτηκα να σ' αρνηθώ).

[3][4] In May 2005, Psarantonis performed at the World Music Institute's 20th anniversary benefit concert at Town Hall, New York.

In January 2009, he gave memorable performances in the rock music festival All Tomorrow's Parties hosted in Brisbane, Sydney and Mount Buller (in Victoria) and curated by Nick Cave & The Bad Seeds.

In 2007 he worked with Daemonia Nymphe on their album Krataia Asterope doing the vocals and playing the lyra in the track Dios Astrapaiou He has also worked with Italian singer and songwriter Vinicio Capossela, similarly to his son Labis.