Ordered assemblies of nanoparticles remain challenging to fabricate, yet could open the door to many potential applications of nanomaterials. Here, we demonstrate that locally ordered arrays of nanoparticles, using electrophoretic deposition, can be extended to produce long-range order among the constituents. Voronoi tessellations along with multiple statistical analyses show dramatic increases in order compared with previously reported assemblies formed through electric field-assisted assembly. Based on subsequent physical measurements of the nanoparticles and the deposition system, the underlying mechanisms that generate increased order are inferred. (C) The Author(s) 2015. Published by ECS.