The impact of adding diatomite on the treatment performance of slightly polluted algae-containing raw water using ozone pre-oxidation and polyaluminum chloride (PAC) coagulation was investigated. Results demonstrated that the addition of diatomite is advantageous due to reduction of the PAC dose (58.33%) and improvement of the removal efficiency of algae, turbidity, and dissolved organic matter (DOM) in raw water. When the ozone concentration was 1.0 mg L⁻¹ and the PAC dosage was 2.5 mg L⁻¹, the removal rates of algae, turbidity, UV254, and TOC were improved by 6.39%, 7.06%, 6.76%, and 4.03%, respectively, with the addition of 0.4 g L⁻¹ diatomite. It has been found that the DOM presented in the Pearl River raw water mainly consisted of small molecules (<1 kDa) and large ones (> 50 kDa). After adding diatomite (0.4 g L⁻¹), the additional removal of 5.77% TOC and 14.82% UV254 for small molecules (<1 kDa) of DOM, and 8.62% TOC and 7.33% UV254 for large ones (>50 kDa) could be achieved, respectively, at an ozone concentration of 1.0 mg L⁻¹ and a PAC dose of 2.5 mg L⁻¹. The growth of anabaena flos-aquae (A.F.) was observed by an atomic force microscope (AFM) before and after adding diatomite. AFM images demonstrate that diatomite may have a certain adsorption on A.F.