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Line a 13-by-9-inch baking pan with parchment paper, foil, or plastic wrap. If using one of the later two, lightly butter or mist with cooking spray.
Place popcorn in a very large mixing bowl and set aside.
Melt butter and sugar together in a saucepan over medium-high heat, stirring occasionally, until mixture begins to boil and butter no longer appears separated.
Add mini marshmallows and stir until melted and smooth.
Pour hot marshmallow mixture over popcorn, stirring and folding popcorn until evenly coated with marshmallow.
Pour into prepared baking pan, and press into an even layer (it might help to butter your hands and use that to press the mixture into the pan, but be careful as the popcorn is still warm).
Let cool for 30 minutes to 1 hour, then remove block of popcorn bars and transfer to a cutting board.
Cut into 24 even squares; drizzle with melted chocolate.
Popcorn bars are best enjoyed within 1-2 days, stored in an airtight container.