Starch makes up more than half of the calories in the human diet and is also a valuable bulkcommodity that is used across the food, brewing and distilling, medicines and renewablematerials sectors. Despite its importance, our understanding of how plants make starch,and what controls the deposition of this insoluble, polymeric, liquid crystalline materialremains rather limited. Advances are hampered by the challenges inherent in analyzingenzymes that operate across the solid–liquid interface. Glyconanotechnology, in the formof glucan-coated sensor chips and metal nanoparticles, present novel opportunities toaddress this problem. Herein, we review recent developments aimed at the bottom-upgeneration and self-assembly of starch-like materials, in order to better understand whichenzymes are required for starch granule biogenesis and metabolism.