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An eco-friendly photocatalytic coating, active under a cost-effective near-visible LED system, was synthesized without any calcination step for the removal of organic pollutants. Three types of doping (Fe, N and Fe + N), with different dopant/Ti molar ratios, were investigated and compared with undoped TiO2 and the commercial P25 photocatalyst. Nano-crystalline anatase-brookite particles were successfully produced with the aqueous sol-gel process, also at a larger scale. All samples displayed a higher visible absorption and specific surface area than P25. Photoactivity of the catalyst powders was evaluated through the degradation of p-nitrophenol in water under visible light (>400 nm). As intended, all samples were more performant than P25. The N-doping, the Fe-doping and their combination promoted the activity under visible light. Films, coated on three different substrates, were then compared. Finally, the photoactivity of a film, produced from the optimal N-Fe co-doped colloid, was evaluated on the degradation of (i) p-nitrophenol under UV-A light (365 nm) and (ii) rhodamine B under LED visible light (395 nm), and compared to undoped TiO2 film. The higher enhancement is obtained under the longer wavelength (395 nm). The possibility of producing photocatalytic films without any calcination step and active under low-energy LED light constitutes a step forward for an industrial development.