The actor is survived by his wife and two daughters, one of whom is upcoming actress Ann Augustine.
His funeral will be held Friday.
Beginning his acting career through theatre, Augustine entered the Malayalam film industry in the mid eighties and since then he has acted in more than 100 films.
Augustine suffered a stroke in 2010 and since then even though not fully fit, he acted in a few films.
Recently his health deteriorated further and was hospitalised frequently. Even though never a front line actor, Augustine excelled when he acted alongside superstars Mammootty and Mohanlal.
Notable among his films were 'Commissioner', 'Devasuram', 'Ekalavyan', 'Aaran Thampuran', 'Kazhcha' and 'Katha Paryumbol'.
His last film was 'Shutter' that was released early this year.
Prominent director Renjith kept him company all through his career and was seen in every film of his.
"He did not become an actor overnight. Instead he made use of small roles that came his way and peaked...he had extremely talented film professionals as his close friends," said Innocent, the president of the actor's body, AMMA.
Photos: Aamir Khan with brother Faisal, ex-wife Reena Dutta at MAMI
Photos: Sonakshi Sinha, Sushant Singh Rajput at Mumbai airport
Spotted: Ajay Devgn and Kajol at an event in Mumbai
Birthday special: 21 cricketers who made their Test debut as teenagers
Pics: Prabhas, Tamannaah Bhatia at 'Baahubali 2' first look launch at MAMI