Large-size cesium triborate (CsB3O5:CBO) crystals were grown from self-flux solutions by top-seeded solution growth. The crystals have numerous scattering centers that were found to depend on the temperature from which the crystals were grown. The weight loss measurements revealed that more weight loss occurred at the growth temperature of 74 mol%B2O3. During the cooling process (after growth) there is a possibility of the crystal being shifted to the off-stoichiometric composition because of cesium out-diffusion. To bring the crystals to near stoichiometric solutions, the vapor transport equilibration (VTE) process (post-growth heat treatment) was carried out and the scattering centers were reduced. The cesium atmosphere used in VTE processing was very important for the diffusion of cesium into the crystal and to bring the crystals to near stoichiometric composition.