The application of doped HfO2 ferroelectric thin films in nonvolatile memory devices becomes popular in condensed matter physics and materials science. Recent studies indicate that La doped HfO2 has excellent ferroelectric properties, and the ferroelectric remanent polarization is 45 μC/cm2 as the maximum value reported. Nd doping is expected to enhance the ferroelectric properties of HfO2 due to its similar chemical properties of Nd and La, but little research has been reported. In this paper, high quality Nd-doped HfO2 (i.e., Nd:HfO2) thin films were grown on La0.67Sr0.33MnO3 (bottom electrode)/SrTiO3 (001) substrates by using oxide molecular beam epitaxy. According to the results by X-ray diffraction and high-resolution electron microscopy, Nd doping can induce the transition of HfO2 from a monoclinic phase to an orthorhombic phase. In addition, the results by high resolution electron microscopy also show that Nd:HfO2 has a tetragonal phase structure near the interface, connecting (111) crystalline Nd:HfO2 and (001) crystalline perovskite oxide substrates. The systematic studies on epitaxial growth and ferroelectric properties of Nd:HfO2 films can expand the research of doped HfO2.