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Preheat oven to 275°F. Grease a large shallow roasting pan; set aside. Combine popcorn and sunflower kernels in a large bowl; set aside.
Combine butter and chocolate in a large saucepan. Heat and stir over medium-low heat until melted. Stir in marshmallows; heat and stir until melted and smooth. Remove from heat. Stir in vanilla.
Pour chocolate mixture over popcorn mixture; stir to coat. Spread popcorn mixture in the prepared pan.
Bake for about 20 minutes or until crisp, stirring once. Cool in pan on a wire rack. Break mixture into pieces.