Falco, 31, moves from Mustoe Merriman Levy, which he joined at the end of last year.
His appointment sees him reunite with the former Lowe creatives Charles Inge, Micky Tudor and Brian Turner.
Falco worked at Lowe for three years before moving with Andy Amadeo and Mick Mahoney to CDP as its head of TV in June 2001. He subsequently moved with them to MML, when CDP handed the creative reins to Gill Sully.
Inge said: "At Lowe he was a young star. He is very good at making ads better and has been associated with a lot of Lowe's best recent work."
He added that Falco has worked successfully with Tudor and Turner on many projects at Lowe, including the Reebok "belly" ad and "old man" for Heineken.
Tudor, Turner and Falco's first work at CHI will be the agency's debut for Heineken, shot by Traktor through Partizan. The agency took the account from Lowe in June.