We demonstrate a facile technique to electrophoretically deposit homogenous assemblies of single-walled carbon nanohorns (CNHs) from common solvents such as acetone and water onto nearly any substrate including insulators, dielectrics, and three-dimensional metal foams, in many cases without the aid of surfactants. This enables the generation of pristine film-coatings formed on time scales as short as a few seconds and on three-dimensional templates that enable the formation of freestanding polymer-CNH supported materials. As electrophoretic deposition is usually only practical on conductive electrodes, we emphasize our observation of efficient deposition on nearly any material, including nonconductive substrates. The one-step versatility of deposition on these materials provides the capability to directly assemble CNH materials onto functional surfaces for a broad range of applications. In this manner, we utilized as-deposited CNH films as conductometric gas sensors exhibiting better sensitivity in comparison to equivalent single-walled carbon nanotube sensors. This gives a route toward scalable and inexpensive solution-based processing routes to manufacture functional nanocarbon materials for catalysis, energy, and sensing applications, among others.