In this study, nano-sized fullerene C60 powder was sufficiently mixed with Cu2SnSe3 powder by ball milling method, and the C60/Cu2SnSe3 composites were prepared by spark plasma sintering technology. The fullerene C60 distributed uniformly in the form of clusters, and the average cluster size was less than 1 ?m. With increasing C60 content, the electrical conductivity of C60/Cu2SnSe3 composites decreased, while the Seebeck coefficient was enhanced. The thermal conductivity of composites decreased significantly, which resulted from the phonon scattering by the C60 clusters located on the grain boundaries of the Cu2SnSe3 matrix. The highest figure of merit ZT of 0.38 was achieved at 700 K for 0.8% C60/Cu2SnSe3 composite.