3D nanosystems equipped with polysulfates as binding sites are effective virus inhibitors due to their ability to dynamically deform while adhering to a virus. Here we present a new supramolecular nanosystem assembled from block copolymer consisting of sulfated linear polyglycerol and polytrimethylene carbonate. It exhibits a unique morphology, 100 nm sized spheres with a distinct brush-like corona. The negatively charged sulfates are distributed on the outer shell and enable exceptional homogeneity of the particles, thereby enhancing the efficiency of multivalent interactions. We tested various sulfation levels and demonstrated extremely low halfmaximal inhibition concentration (IC50) values in plaque reduction assays tested on HSV-1: 0.43 mg/mL, 0.16 mg/mL and 0.037 mg/mL of the 45%, 76% and 100% sulfated assemblies, respectively. Using cryo-EM we observed viruses trapped by multiple layers of the nano-assemblies. Both 76% and 100% sulfated assemblies showed therapeutic potential in the post-infection model. We further confirmed the inhibitory behavior of the 76% and 100% sulfated assemblies against Omicron infection. Our work demonstrates that the presented 3D flexible nano-assemblies can block the virus entry into the host cells with superior morphology and efficiency, establishing them as a promising candidate for antiviral applications.