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Mesoporous TiO 2 films with enhanced photocatalytic activity in both UV and visible wavelength ranges were developed through a non-conventional atomic layer deposition (ALD) process at room temperature. Deposition at such a low temperature promotes the accumulation of by-products in the amorphous TiO 2 films, caused by the incomplete hydrolysis of the TiCl 4 precursor. The additional thermal annealing induces the fast recrystallisation of amorphous films, as well as an in situ acidic treatment of TiO 2 . The interplay between the deposition parameters, such as purge time, the amount of structural defects introduced and the enhancement of the photocatalytic properties from different mesoporous films clearly shows that our easily upscalable non-conventional ALD process is of great industrial interest for environmental remediation and other photocatalytic applications, such as hydrogen production., Competing Interests: There are no conflicts of interest to declare., (This journal is © The Royal Society of Chemistry.)