Prepare outdoor grill with medium-hot coals, or heat gas grill to medium-high, or see Stovetop Method, below.
Toast pound cake on grill about 2 minutes per side. Remove from grill. Spread each of 6 slices with 2 tablespoons marshmallow cream. Place 1 of the chocolate squares on top of cream. Top each with a slice of remaining pound cake.
Place each of smores over indirect heat until chocolate starts to melt, 1 minute or less. Serve immediately. Makes 6 servings.
Heat stovetop grill pan over medium-high heat. Place pound-cake slices on pan; toast, about 2 minutes per side. Proceed with steps 2 and 3 above.