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Achieving ordered arrays of nanoparticles (NPs) with controlled packing symmetry and interparticle spacing is of great importance to design complex metamaterials. Herein, we report softness- and size-dependent self-assembly behavior of polystyrene-grafted Au NPs (Au@PS NPs). We varied the core size of Au NPs from 1.9 to 9.6 nm and the number-average molecular weight (Mn) of thiol-terminated polystyrene from 1.8 to 7.9 kg mol-1. The optimal packing model based on an "effective softness" parameter λeff that accounts for close-packed and se