Put 1/3 cup of the sugar and the orange zest in a small bowl. Stir until blended and set aside.
Arrange a large piece of plastic wrap on the counter. Using a rolling pin, roll out the puff pastry on the plastic into a 10 x 15-inch rectangle. Sprinkle the top and bottom often and generously with the remaining 1/3 cup sugar to prevent sticking (you won’t use it all). Pour the melted butter onto the center of the dough and spread evenly with a small offset spatula. Sprinkle the reserved sugar-orange mixture evenly over the butter.
Cut the dough in half crosswise (you’ll have two 10 x 71/2-inch rectangles). Starting on one short side and using the plastic as a guide, roll up the dough jellyroll style to the center. Roll up the opposite side until the 2 rolls meet in the center. Pinch the rolls so they stick together. Repeat with remaining dough. Wrap the rolls and refrigerate until firm, about 45 minutes (for faster chilling, pop the wrapped rolls in the freezer).
Heat the oven to 425°F. Line 2 large cookie sheets with nonstick liners.
Arrange the rolls, seam side down on a cutting board and cut into 1/2-inch-thick slices. Arrange on the prepared cookie sheets about 1-1/2 inches apart. Bake until golden brown, about 14 minutes. Turn over and bake for another 1 to 2 minutes until golden brown. Set on a rack to cool completely. Serve immediately or cover and store at room temperature for up to 2 days.