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Thermoelectrics (TEs) are an important class of technology that harvest electric power directly from heat sources. When designing both high performance and environmentally friendly TE materials, the pseudo-cubic structure has great theoretical potential to maximize the dimensionless figure of merit ZT . The TE multinary single crystal with a pseudo-cubic structure paves a new path toward manipulating valley degeneracy and anisotropy with low thermal conductivity caused by short-range lattice distortion. Here, we report a record high ZT = 1.6 around 800 K realized in a totally environmentally benign p-type Na-doped Cu 2 ZnSnS 4 (CZTS) single crystal. The exceptional performance comes from a high power factor while maintaining intrinsically low thermal conductivity. The combination of the pseudo-cubic structure and intrinsic properties of the CZTS single crystal takes advantage of simple material tuning without complex techniques.