A universal environmental friendly method was developed to turn sand into effective flocculants for mitigating harmful algal blooms (HABs) in marine and freshwater systems. The isoelectric point of sand was largely increased from pH 4.5 to 10.5 after been modified by Moringa oleifera coagulant (MO) abstracted form MO seeds. However, when sand was modified by MO alone, maximum removal efficiencies of 80% and 20% for Amphidinium carterae (A.C.) and Chlorella sp. (C.S.) in seawater and 60% for Microcystis aeruginosa (M.A.) in fresh water were achieved in 30 min. The limited removal improvement was due to the form of only small flocs (20-100 μm) by surface charge modification only. Large flocs (270-800 μm) and high removal rate of 96% A.C. and C.S. cells in seawater and 90% of M.A. cells in fresh water were achieved within 30 min when the small MO-algae-sand flocs were linked and bridged by chitosan. High HAB removal rate is achievable when the sand is modified by the bicomponent mechanism of surface charge and netting-bridging modification using biodegradable modifiers such as MO and chitosan. The optimized dosage of modified sand depends on the property of algal cells and water conditions.