A convenient route was developed for the selective preparation of two stable nanocomposites, Ti3+/TiO2/CNT (labeled as TTOC-1 and TTOC-3) and Ti3+/TiO2/carbon layer (labeled as TTOC-2), from the same precursor by varying the amount of single-walled carbon nanotubes used in the synthesis. TiO2 is an effective photocatalyst; however, its wide bandgap limits its usefulness to the UV region. As a solution to this problem, our prepared nanocomposites exhibit a small bandgap and wide visible-light (VL) absorption because of the introduction of carbonaceous species and Ti3+ vacancies. The photocatalytic efficiency of the nanocomposites was examined via the degradation of methylene blue dye under VL. Excellent photocatalytic activity of 83%, 98%, and 93% was observed for TTOC-1, TTOC-2, and TTOC-3 nanocomposites within 25 min. In addition, the photocatalytic degradation efficiency of TTOC-2 toward methyl orange, phenol, rhodamine B, and congo red was 28%, 69%, 71%, and 91%, respectively, under similar experimental conditions after 25 min. Higher reusability and structural integrity of the as-synthesized photocatalyst were confirmed within five consecutive runs by photocatalytic test and X-ray diffraction analysis, respectively. The resulting nanocomposites provide new insights into the development of VL-active and stable photocatalysts with high efficiencies.