Micro-Vickers hardness of LaB6, La0.7Ce0.3B6, La0.82Pr0.18B6 and La0.85Nd0.15B6 crystals was measured from room temperature to 1300-degrees-C. The rare-earth substituted LaB6 Crystals were confirmed to be boundary-free as a result of solid solution hardening. In addition, the hardness measurement revealed that boundary-free LaB6 Crystals can be prepared when the growth temperature is decreased to temperatures 200-degrees-C below the melting point, which agreed well with the experimental results by the traveling solvent floating zone method.