Writer-director Marc Abraham's movie will chronicle the country music icon's rise to international fame, and his death at age 29 after years of alcohol abuse, reported Variety.
Olsen has been cast as Williams's wife Audrey Mae.
Production on the movie - which is based on the book Hank Williams: The Biography - will begin in Louisiana next month.
Olsen recently starred in the blockbuster 'Godzilla', and will soon play the Scarlet Witch in Marvel's 'Avengers: Age of Ultron'.
Hiddleston is also a contributor to the Marvel Cinematic Universe, having portrayed the villain Loki in 'The Avengers' and both 'Thor' films.
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