Abstract: Here, we report on hierarchical mechanical behavior of 500-nm-thick Co-nanocrystal 3D superlattices (supracrystals) induced by either the crystalline structure (nanocrystallinity) or the length of the coating agent of Co nanocrystals. Increasing the nanocrystal shape anisotropy of Co nanocrystals through the control of their nanocrystallinities induces a higher level of ordering with both translational and orientational alignment of nanocrystals within the supracrystals.