Puncture the eyes on the end of the coconut and drain the liquid inside. Save the liquid (known as coconut milk) for another use if desired.
Using a mallet or hammer, tap the shell all around to loosen the meat inside. Break the coconut open, using the same tool. Remove the meat from the shell by inserting a table knife between the meat and shell. Use a vegetable peeler or a sharp knife to remove the brown skin from the meat, leaving it in large pieces. Rinse the coconut pieces.
Using a mandoline, slice the coconut pieces against the grain into strips 1/16 inch (2 mm) thick and as long as possible. They break fairly easily, so you will most likely have shavings about 1 to 2 inches (2.5 to 5 cm) long. Cutting against the grain will make for curved strips, which hold together better and are more attractive. Do not mix slices of differing thickness on the same baking pan, as it makes it very hard to bake them evenly. If it takes a few tries to adjust the mando-line to the proper thickness, discard the trial slices.
Place the slices in a bowl and add enough simple syrup to coat the pieces with syrup, mixing them with your fingers. Place the slices on Silpats in a single layer.
Bake at 325°F (163°C) for 15 to 20 minutes or until the slices are golden. If they appear dry during the baking process, brush additional simple syrup on top to keep them moist. Remove from the oven and use 2 forks to transfer the chips to a cold nonstick surface, keeping them separate so they don’t stick together. The chips will cool and become crisp almost immediately and can then be stored in an airtight container.