This work aims to study the effect of pulse power supply on the formation of TiO2 nanotubes and their photocatalytic properties under different voltage and duty cycles in the pulse mechanism. A pulsed power supply was used to prepare TiO2 nanotubes on the surface of pure titanium substrates with different pulse voltages and duty cycles. The surface morphology and composition of the nanotube were analyzed by SEM and EDS. By optimizing the voltage and duty cycle parameters, we obtained TiO2 nanotubes with good shapes, which were used to explore their photocatalytic degradation of methyl orange. When the pulse voltage was increased from 50 V to 80 V with a duty cycle of 15%, TiO2 nanotubes showed high quality, and the tube diameter was increased with the increasing voltage. The methyl orange solution was degraded by 21.2% after 6 h xenon lamp irradiation. The results show that TiO2 nanotubes prepared by pulse voltage anodic oxidation can degrade methyl orange by photocatalysis.