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To improve the visible light absorption and photocatalytic activity of titanium dioxide nanotube arrays (TONTAs), ZnFe2O4(ZFO) nanocrystals were perfused into pristine TONTA pipelines using a novel bias voltage-assisted perfusion method. ZFO nanocrystals were well anchored on the inner walls of the pristine TONTAs when the ZFO suspensions(0.025 mg mL-1)were kept under a 60 V bias voltage for 1 h. After annealing at 750?C for 2 h, the heterostructured ZFO/Fe2TiO5(FTO)/TiO2com-posite nanotube arrays were successfully obtained. Fur-thermore, Fe3?was reduced to Fe2?when solid solution reactions occurred at the interface of ZFO and the pristine TONTAs. Introducing ZFO significantly enhanced the visible light absorption of the ZFO/FTO/TONTAs relative to that of the annealed TONTAs.The coexistence of type I and staggered type II band alignment in the ZFO/FTO/TONTAs facilitated the separation of photogenerated electrons and holes,thereby improving the efficiency of the ZFO/FTO/TONTAs for photocatalytic degradation of methylene blue when irradiated with simulated sunlight.