Nd3Te4 crystallizes in the cubic I-43d space group. The structure is three-dimensional. Nd+2.67+ is bonded to eight equivalent Te2- atoms to form a mixture of distorted edge, face, and corner-sharing NdTe8 hexagonal bipyramids. There are four shorter (3.22 Å) and four longer (3.39 Å) Nd–Te bond lengths. Te2- is bonded to six equivalent Nd+2.67+ atoms to form a mixture of distorted edge, face, and corner-sharing TeNd6 octahedra. The corner-sharing octahedra tilt angles range from 17–50°.