We present an approach utilizing ion assisted aerosol lithography (IAAL) with a newly designed multi-pin spark discharge generator (SDG) for fabricating large-area three-dimensional (3D) nanoparticle-structure (NPS) arrays. The design of the multi-pin SDG allows us to uniformly construct 3D NPSs on a large area of 50 mm × 50 mm in a parallel fashion at atmospheric pressure. The ion-induced focusing capability of IAAL significantly reduces the feature size of 3D NPSs compared to that of the original pre-patterns formed on a substrate. The spatial uniformity of 3D NPSs is above 95% using the present multi-pin SDG, which is far superior to that of the previous single-pin SDG with less than 32% uniformity. The effect of size distributions of nanoparticles generated via the multi-pin SDG on the 3D NPSs also has been studied. In addition, we measured spectral reflectance for the present 3D NPSs coated with Ag, demonstrating enhanced diffuse reflectance.