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Hexavalent chromium Cr(VI) pollution makes has a harmful impact on human health and the ecological environment. Photocatalysis reduction technology exhibits low energy consumption, high reduction efficiency and stable performance, and is playing an increasingly important role in chromium pollution control. Graphite-phase carbon nitride has been used to reduce Cr(VI) to the less harmful Cr(III) due to its visible light catalytic activity, chemical stability and low cost. However, it has a low specific surface area and fast recombination of electron–hole pairs, which severely restrict its practical application. In this work, a TiO2-modified poly(triazine imide) (PTI) square nanotube was prepared by the one-step molten salts method. The results showed the PTI had a square hollow nanotube morphology, with an about 100–1000 nm width and 60–70 nm thickness. During the formation of the PTI square tube, TiO2 nanoparticles adhere to the surface of the square tube wall by strong adsorption, and eventually form a PTI/TiO2 heterojunction. The PTI/TiO2-7 wt% heterojunction exhibited very good Cr(VI) reduction efficiency within 120 min. The enhanced photocatalytic activity was mainly attributed to the efficient separation and transport of photo-induced electron–hole pairs and the high specific surface area in the heterojunction structure.