In this study, a series of TiO2 nanotubes (NTs) were synthesized employing electrochemical anodization of titanium foil in an ionic liquid solution containing a mixture of glycerol and choline chloride, acting as electrolyte. The as-synthesized TiO2 NTs were calcined at 350, 450, or 550 °C for a 2 h duration to investigate the influence of calcination temperature on NTs formation, morphology, surface properties, crystallinity, and subsequent photocatalytic activity for visible light photodegradation of gaseous formaldehyde (HCHO). Results showed that the calcination temperature has a significant effect on the structure and coverage of TiO2 NTs on the surface. Freshly synthesized TiO2 NTs showed better-ordered structure compared to calcined samples. There was significant pore rupture with increasing calcination temperature. The transformation from anatase to rutile phase appeared after calcination at 450 °C and the weight fraction of the rutile phase increased from 19% to 36% upon increasing the calcination temperature to 550 °C. The band gaps of the TiO2 NTs were in the range from 2.80 to 2.74 eV, shifting the active region of the materials to visible light. The presence of mixed anatase–rutile TiO2 phases in the sample calcined at 450 °C showed enhanced photoactivity, which was confirmed by the 21.56 mg∙L−1∙g−1 removal of gaseous formaldehyde under 120 min of visible light irradiation and displayed enhanced quantum yield, ∅HCHO of 17%.