addressing challenges associated with clean energy generation and environmental pollution. [1][2][3][4][5] For TiO 2 based catalysts, materials in the form of solid films are particularly desirable since this addresses one of the most important problems associated with traditional photocatalyst systems, which is that powder-like TiO 2 photocatalysts tend to agglomerate and are difficult to recover. [6] Of particular interest is solid TiO 2 films that are flexible, robust, and transparent since this would greatly facilitate the actual use of these photocatalysts under real-life conditions where the surface of interest is curved and/or the reaction container is irregular.In our previous research we have developed a one-pot self-assembly method that allows such films to be produced which contain only single layers of TiO 2 nanoparticle (NP) clusters firmly anchored on a flexible and lightweight polystyrene support. [7] Importantly, unlike traditional methods for self-assembly, which often involve the use of modifying ligands that adsorb strongly to the surface of the NP catalysts, our method allows photo-catalytically active TiO 2 NP powder to be assembled directly into densely packed monolayer films without introducing ligands onto the TiO 2 surface. [8][9][10][11][12] In this material, molecules have unrestricted access to the catalytic TiO 2 surface, which is a prerequisite for photocatalysts to exhibit high photocatalytic activity. [13] These films are therefore called "surface exposed nanoparticle sheets", namely SENSs.While this assembly process addresses the handling issues associated with using TiO 2 as a photocatalyst and creates a material that is very suitable for real world applications, the efficiency of the material is still determined by the properties of the photocatalyst itself, which in the case of TiO 2 is limited by the fast recombination of the electron-hole pairs created by UV excitation. [14][15][16] A widely adopted strategy to address this issue is to prepare hybrid metal-TiO 2 nanomaterials. Since metals such as Au and Pt have larger work functions than TiO 2 , electrons flow from TiO 2 to metals when they are in close contact, leading to the formation of Schottky barrier which prohibits the backflowing of photogenerated electrons when TiO 2 is excited. [17,18] This effectively prolongs the lifetime of electron-hole pairs andThe photocatalytic efficiency of TiO 2 can be increased by using co-catalysts, such as metal nanoparticles, which act as electron sinks to suppress the recombination of photogenerated electron-hole pairs. The main challenge in preparing such systems is to create intimate contact between the metal and the TiO 2 surface while still maintaining control over the morphology and distribution of the metal nanoparticles in the TiO 2 matrix. Here lightweight TiO 2 films are prepared by assembling a layer of TiO 2 nanoparticles onto a thin polymer support, followed by physical vapor deposition of metal nanoparticles onto the TiO 2 surface. Importantly the fabrication does not inv...