Gd-doped TiO2 nanotube arrays with 3D ordered and high specific surface (176 m2/g) area are successfully prepared on a Ti foil surface via an anodizing method. The characterizations of Gd-doped TiO2 nanotube arrays are carried out using X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscope (TEM), X-ray photoelectron spectroscopy (XPS), energy dispersive X-ray spectrometer (EDX), optical contact angle measurer, and ultraviolet (UV) fluorescence spectrophotometer, respectively. The results reveal that the Gd-doped TiO2 nanotube arrays form on the Ti foil surface with a length of about 50.5 μm and 100 nm in diameter, and the growth direction grown along the (101) direction of anatase crystal. Under the optimized reaction conditions (60 V, 10 h, 0.01mol/L Gd3+), the crystal phase of Gd-doped TiO2 show an excellent nanotube structure, possess a beneficial photocatalytic performance for methyl orange (MO) (Degradation rate was 95.8%) and an excellent hydrophilic property (The optical contact angle was 4.9°). After doping with Gd, the hydrophilic and photocatalytic properties of the TiO2 nanotubes are further improved.