Pentaerythritol (PET) crystal has been grown rapidly from the solution with sulfuric acid as the additive. The growth rate of PET crystal in prismatic shape exceeds 1.5 mm/day and crystallization size is 55 × 55 × 50 mm3. X-ray diffraction analysis was used to confirm the structure integrity. The diffraction efficiency of rapid-grown crystal was characterized as effective as that of normal growth.