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The Last Station is based on Jay Parini's 1990 novel of the same name, which covers the turbulent last year of the Russian writer's life.
Plummer will play Tolstoy and Mirren will be his wife Sofia, replacing Anthony Hopkins and Meryl Streep, who were previously announced in the roles.
The Michael Hoffman-directed movie also stars James McAvoy and Paul Giamatti.
Production is scheduled to begin in Germany next week.
Plummer is currently shooting The Imaginarium of Doctor Parnassus, the film Heath Ledger was working on before his death.
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