Electrochromic (EC) materials change their optical properties (darken/lighten) in the presence of a small electric potential difference, and are suitable for application in energy-efficient windows, antiglare automobile rear-view mirrors, sunroofs, displays, and hydrogen sensors. [1][2][3][4] There are two important criteria for selecting an EC material. The first is the time constant of the ion-intercalation reaction, which is limited both by the diffusion coefficient and by the length of the diffusion path. While the former depends on the chemical structure and crystal structure of the metal oxide, the latter is determined by the material's microstructure. [11] In the case of a nanoparticle, the smallest dimension is represented by the diffusion path length. Thus, designing a nanostructure with a small radius, while maintaining the proper crystal structure, is key to obtaining a material with fast insertion kinetics, enhanced durability, and superior performance. The second important criterion is coloration efficiency (CE), the change in optical density (OD) per unit inserted charge (Q), that is, CE = D(OD)/DQ. [12] A high CE provides large optical modulation with a small charge insertion or extraction. This is a crucial parameter for EC devices, since a lower charge-insertion or -extraction rate enhances the longterm cycling stability. Among inorganic materials, tungsten oxides have been most extensively studied. Up until now, amorphous WO 3 films have exhibited the highest CE in the visible region of the electromagnetic spectrum. However, because of their high dissolution rate in acidic electrolyte solutions, these films can only be used in lithium-based electrolytes, resulting in slower response times. Furthermore, extended durability, even in Li + systems, has not yet been demonstrated. Inexpensive conducting and redox polymers have attracted increased attention for use as EC materials because of their fast response times and high contrast ratios. [13][14][15] However, disadvantages include multiple coloration in the visible spectral range and poor UV stability. By fabricating EC films from crystalline WO 3 nanoparticles, the state-of-the-art technology of producing EC materials has been profoundly advanced. Crystalline WO 3 nanoparticles have been grown by an economical hot-wire chemical-vapordeposition (HWCVD) process, and a unique electrophoresis technique is employed for the fabrication of porous nanoparticle films. The porosity of the films not only increases the surface area and ion-insertion kinetics, but also reduces the overall material cost, leading to an inexpensive, large-area EC material. Compared to conventional amorphous WO 3 films prepared by vacuum deposition, nanoparticle films deposited by electrophoresis exhibit vastly superior electrochemical-cycling stability in acidic electrolytes, a higher charge density, and comparable CE. This greatly enhanced stability and charge capacity are attributed to the crystalline nanoparticles employed in this work. These initial results will ultimately ...