Lanthanide-doped upconversion nanoparticles (UCNPs) can absorb near-infrared photons and convert them into visible and ultraviolet emissions. These nanomaterials possess extraordinary optical perfor-mance and hold potential as active platforms for a variety of technological applications. The ability to fabricate highly ordered nanoparticle-based photonic elements over a large area is of fundamental sig-nificance for luminescence tuning. Despite all the efforts made, however, large-area spatial patting of UCNPs into ordered arrays with high controllability remains a challenge. In this study, we report a high-throughput strategy to patt optical nanomaterials through the use of polymer microspheres and templated assembly of UCNPs. This technique utilizes capillary force to drive hybrid clusters into the physical template, resulting in large-area, spatially ordered arrays of particles. The findings reported in this work may promote the development of novel nonlinear optical devices, such as solid-state laser arrays, high-density optical storage, and anti-counterfeiting labels.