Nanocrystalline diamond nanomembranes with thinning-reduced flexural rigidities can be shaped into various 3D mesostructures, such as tubes, jagged ribbons, nested tubes, helices, and nested rings. Microscale helical diamond architectures are formed by controlled debonding in agreement with finite-element simulation results. Rolled-up diamond tubular microcavities exhibit pronounced defect-related photoluminescence with whispering-gallery-mode resonance.