Surface modification of ceramic Ce-doped Gd3Al2Ga3O12 (Ce:GAGG) was performed by exposing small samples to anhydrous phosphoric acid (H3PO4) under different conditions (temperature and duration) to investigate the effects of chemical polishing treatment. When coupled to a photomultiplier tube (PMT) and used as a radiation detector, chemical treatment for 3 min at 190 °C improved the light (signal) output by 24.8% and energy resolution by 2.5% (percentage point), respectively. This can be attributed to a reduction in surface roughness that enhanced optical properties. Thus, chemical polishing could be a low-cost alternative to mechanical polishing especially for small or complex shaped ceramic scintillators.