Hierarchical porous acrylate‐based materials are highly interesting as 3D filter materials, such as for virus removal from suspensions. Here, the synthesis of highly porous monolithic 3D materials by polymerization‐induced phase separation in liquid crystal display (LCD) based 3D printing is presented for the efficient removal of human adenovirus type 5. The hierarchical porosity can be tuned via the variation of the photocurable resin composition (i.e., inherent porosity) and the computer‐aided design (i.e., “printed” porosity; microchannels). 3D polymer structures with highly intricate geometries and structural features ranging from ≈20 nm up to cm can be achieved, which can be used for effective virus removal in a laboratory‐scale flow‐through approach. Combined focused ion beam/scanning electron microscopy tomography and mercury porosimetry provide detailed information on the inherent pore size, pore size distribution, and pore interconnectivity, which is key for the performance of such functional 3D materials. Polymers with a theoretical void volume of 75% show virus capture with a removal efficiency of ≈70% of the adenovirus. Polymers with the same theoretical void volume and macroscopic design but a more hydrophobic nature captured only ≈33%. An optimized adenovirus retention of 98% is achieved by adjusting the microchannels of the tunable inserts.