The 36-year-old World Cup winner took over in June, but stepped down immediately following a 3-2 home defeat by Asteras Tripolis.
“I have put all my passion and all my strength into this team but I can’t be the one solving all the club’s problems every day, I’m not the president and my job should only be football,” Gattuso told a news conference.
“I feel very upset but I cannot continue. The players don’t believe in me.”
He had a previous colourful rant criticising the players and club which became a YouTube hit.
Gattuso, who won 73 caps and helped Italy lift the World Cup in 2006 as well as sealing two Champions League titles with
Milan, succeeded Portuguese Ricardo Sa Pinto after he led the unfancied team to sixth last term.
But OFI have struggled with inconsistent form this term, with this latest setback leaving the Crete club in mid-table with nine points from seven matches.
Gattuso has struggled in his first attempts at managing, with his first job at Swiss club FC Sion ending with him being sacked, before a spell at Palermo ended after three patchy months.