Gravity enables self‐assembly

Abstract Crystallization of granular assemblies has broad implications for rapid and scalable creation architected materials with applications ranging from structural to microarchitected battery electrodes. While significant advances have been made in understanding colloidal self‐assembly at nano micro scale, the governing mechanisms organization dry hard spheres remain unclear. Here, we investigate crystallization mono‐size without imposed vibration. Using X‐ray computed tomographic analysis coupled discrete‐element simulations, unravel roles gravity vibration on three‐dimensional spheres. We use these insights introduce gravity‐mediated epitaxial crystal growth slow pouring balls seeding templates. Contrary vibration‐induced crystallization, this method can form large single crystals both close‐packed rather surprisingly, nonclose‐packed metastable particle arrangements. Our results provide insight manufacture defect‐free that be used as space‐holding templates cellular materials, such inverse opals other related topologies. Key points Self‐assembly is a critical step micro‐architected solids. Via combination experiments, 3D observations, elucidate role design not only induce into stable structures but also counterintuitively structures.