This paper describes the application of electrophoretic deposition for air pollution removal using anatase as a photoactive coating. In this study, the anatase form of TiO2 has been applied to (1) fluorine-doped tin oxide (FTO)-coated glass; (2) 304L stainless steel; and (3) titanium substrates using isopropanol and acetylacetone-based solutions at 20, 40, 60 and 80 V. In order to increase the strength of the substrate–anatase interface without transforming the phase into rutile, samples were calcined at 450 °C for 2 h. The resulting coatings were characterised by Raman spectroscopy, X-ray diffraction, non-contact optical profilometry and scanning electron microscopy. The photocatalytic activity of the deposited coatings were evaluated in the gas phase for nitrogen dioxide (NO2) removal by electron ionisation mass spectrometry, whilst irradiated by light of wavelength 376–387 nm for 100 min. Anatase phase titania supported on a FTO-coated glass substrate showed the highest photoactivity for NO2 remediation. This was attributed to the formation of a three-dimensional nanostructure with properties determined by the deposition conditions. This work provides routes for the development of low-cost and large area photoactive coatings for pollution control.