In a dramatic break from his previous casting as Prince Philip in The Crown, Smith now plays the part of the infamous serial killer who died in November.
Directed by Mary Harron, who made the 2000 Christian Bale film "American Psycho", the film is set three years after the brutal 1969 murders of, among others, Roman Polanski's actress wife Sharon Tate and her unborn child.
Serving life in jail are three women – Susan Atkins, Leslie Van Houten and Patricia Krenwinkel – who are still in thrall to Manson.
Trying to dispel the bizarre delusions that Manson is a God-like figure who will save them, is a prison teacher named Karlene Faith – who tries to get the trio to face up to their murderous actions.
Speaking to Reuters, Harron said: "That's a perspective that no one has seen and no one has really focused entirely on: their story or their journey about how they ended up there and why they did the things they did.
"To me that's the great mystery. You know Charles Manson was insane, but they were not, so how did he get them to do these things?"
Smith, 35, added: "This isn't a film about Charles Manson. There's nothing new to find out (about him), but I like the idea that this was a film about what made these girls go to commit these crimes."
During the murderous rampage on August 9, 1969, the pregnant Tate, Jay Sebring, a celebrity hairstylist, Voytek Frykowski, a screenwriter, and the coffee-fortune heiress Abigail Folger, were horrifically butchered at the home of director Polanski.
Steven Parent, an 18-year-old student, was also shot dead on the driveway to the house.
The next night Manson sent out his deadly crew again – known as "The Family" – and they randomly murdered Leno LaBianca, a grocery-store-chain owner, and his wife Rosemary in their home.
After initially living a bohemian and hippie lifestyle with his mostly female followers in a commune, Manson's warped thinking turned increasingly dark and sinister.
He started viewing himself as Jesus and became obsessed with the Beatles’ White Album, especially the song “Helter Skelter”, which he interpreted as a vision of a coming apocalyptic race war between blacks and whites, from which the Manson Family would emerge as “the chosen people”, with him as their leader.
Screenwriter Guinevere Turner, who co-wrote the "American Psycho" script with Harron, said she wanted to show how easily people could be influenced by a charismatic cult leader such as Manson.
She said: "(I tried) to sort of implicate the audience in 'what would you do?' It was all very fun and happy, and orgies and drugs at the beginning, and that was great.
"And then and it turned and at what part of the journey would you walk away?"
The movie is titled "Charlie Says" as it's the three girls' go-to phrase whenever Karlene questions their ongoing loyalty to Manson.
It premiered at the Venice Film Festival on September 2.
A separate movie about Manson, directed by Quentin Tarantino and starring Australian actor Damon Herriman called "Once Upon a Time in Hollywood", will be released in July next year.
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