Dinoflagellate requires a lower temperature and blooms frequently in the spring and autumn compared to regular cyanobacteria. The outbreak of dinoflagellate bloom will also lead to the death of some aquatic organisms. However, research on freshwater dinoflagellates is still lacking due to the challenges posed by classification and culture in laboratory. The removal effect and mechanism of Peridinium umbonatum (P. umbonatum, a typical dinoflagellate) were investigated using solar/chlorine in this study. The effect of simulated solar alone on the removal of algae was negligible, and chlorine alone had only a slight effect in removing algae. However, solar/chlorine showed a better removal efficiency with shoulder length reduction factor and kmax enhancement factor of 2.80 and 3.8, respectively, indicating a shorter latency period and faster inactivation rate for solar/chlorine compared to solar and chlorine alone. The removal efficiency of algae gradually increased with the chlorine dosage, but it dropped as the cell density grew. When the experimental temperature was raised to 30 °C, algal removal efficiency significantly increased, as the temperature was unsuitable for the survival of P. umbonatum. Attacks on cell membranes by chlorine and hydroxyl radicals (•OH) produced by solar/chlorine led to a decrease in cell membrane integrity, leading to a rise in intracellular reactive oxygen species and an inhibition of photosynthetic and antioxidant systems. Cell regeneration was not observed in either the chlorine or solar/chlorine systems due to severe cell damage or cysts formation. In addition, natural solar radiation was demonstrated to have the same enhancing effect as simulated solar radiation. However, the algal removal efficiency of solar/chlorine in real water was reduced compared to 119 medium, mainly due to background material in the real water substrate that consumed the oxidant or acted as shading agents.