CsB3O5 (CBO) is an excellent nonlinear optical crystal and can be grown by top-seeded solution growth (TSSG) from self-flux solutions. However, there are scattering centers in the as-grown crystal, which decrease the bulk laser-induced damage threshold (LIDT) of the crystal. Postgrowth quenching and vapor transport equilibration (VTE) can reduce the scattering centers effectively. Based on our previous hypothesis and analysis of retrograde solid solution at high temperature in CBO crystal, we adopt selective quenching to 500°C—fast cooling. Our investigations showed that, after the cooling process, the scattering centers and optical loss of CBO were decreased. It was found that with the increase in cooling rate, the LIDT of CBO crystals was increased. The highest LIDT of fast cooling CBO was 1.5 times that of conventional cooling process; so the crystal quality was improved.