Three-dimensional (3D) titanates hierarchical macro/nano-architectures constructed by one-dimensional (1D) nanobelts are successfully synthesized by a hydrothermal-calcining process using metal Ti particles as a precursor. Their morphology and structure are characterized, and their photocatalytic reactivity to tetracycline hydrochloride (TC) is evaluated under visible-light irradiation. The results show that the 1D nanobelts are formed through hydrothermal reaction, and then those 1D nanobelts encircle the metal Ti particles precursor to form 3D macro/nano-architectures. The products with different phase composition, from hydrated titanium oxides to sodium titanates, are obtained by increasing the post-calcining temperatures from 200 degrees C to 800 degrees C. The photocatalytic degradation of TC is observed for all samples under visible-light irradiation, and the sample calcined at 600 degrees C achieves the best photocatalytic reactivity. The visible-light performance of as-synthesized catalysts is considered as a charge-transfer mechanism initiated by the photoexcitation of the surface-complex between TC molecules and titanates, and then followed by the photosensitization mechanism. Two intermediates are identified in the photodegradation process using liquid chromatography combined with mass spectrometry. In addition, the as-synthesized titanates are stable and can be used repeatedly, showing their promising prospect in the practical applications.