The high quality (Ce 0.4 La 0.2 Pr 0.2 Nd 0.2 )B 6 single-crystal has been successfully prepared by the optical float-zone traveling solvent technique. The crystal structure and performance of the (Ce 0.4 La 0.2 Pr 0.2 Nd 0.2 )B 6 single-crystal obtained at different rates are characterized by using XRD, X-ray single-crystal diffraction, rotating target X-ray Diffractometer, X-ray Laue diffraction, SEM and thermionic emission equipment etc.. The results show that the as-grown single-crystal with the uniform composition has a cubic structure with the lattice size of 4.143Å. The optimal mechanical and thermionic emission properties belong to the (Ce 0.4 La 0.2 Pr 0.2 Nd 0.2 )B 6 single-crystal prepared at growth rate V = 7 mm/h. The values of 53.3 A/cm 2 in the current density at 1873 K under the applied voltage of 4 kV and 29.26 GPa in Vickers hardness indicate that (Ce 0.4 La 0.2 Pr 0.2 Nd 0.2 )B 6 single-crystal is a promisingly thermionic emission material.