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Titanium dioxide (TiO 2) as an important semiconductor is widely used in the fields of solar cell, solar thermal collectors, and photocatalysis, but the visible-light power harvest remains insufficient due to the little effective visible-light absorption and many carrier-recombination centers originating from the wide band gap structure. Herein, conductive black titania (BT) nanomaterials with crystalline-TiO 2-core/amorphous-TiO 2−x-shell structure prepared through two-zone Al-reduction route are found efficient in photocatalyzing the degradation of organic pollutants to environmentally friendly products under full solar and even visible light irradiation. The unique core-shell structure and numerous surface oxygen vacancies or Ti 3+ species in the amorphous layer accompanying prominent physicochemical properties of narrow band gap, high carrier concentration, high electron mobility, and excellent separation and transportation of photoinduced e − −h + pairs result in exceptional photocatalytic efficiency. The optimized BT-500 (pristine TiO 2 treated at 500 °C during two-zone Al-reduction process) catalyst achieves superior photocatalytic degradation rates for toluene and ethyl acetate as well as an excellent photostability with high degradation efficiency of 93% for the 6th reuse.