Natural soft materials are often composed of proteins that self-assemble into well-defined structures and display mechanical properties that cannot be matched by manmade materials. These materials are frequently mimicked with hydrogels whose mechanical properties depend on their composition and the type and density of cross-links. Protocols to tune these parameters are well established and routinely used. The mechanical properties of hydrogels also depend on their structure; this parameter is more difficult to control. In this paper, we present a method to produce hexagonal-prismatic granular hydrogel sheets with well-defined structures and heterogeneous cross-link densities. The hydrogel sheets are made of self-assembled covalently cross-linked 40–120 μm diameter hexagonal-prismatic hydrogel particles that display a narrow size distribution. The structure and microscale surface roughness of the hydrogels sheets can be tuned with the polymerization conditions, their chemical composition with that of the individual hydrogel particles, and their mechanical properties with the cross-link density. Remarkably, the hydrogels composed of hexagonal-prismatic microparticles are significantly stiffer than unstructured counterparts. These results demonstrate that the stiffness of hydrogels can be tuned by controlling their micrometer-scale structure without altering their composition. Thereby, they open up new possibilities to design soft materials whose performance more closely resembles that of natural ones.