The flocculation efficiency of microalgae Chlorella vulgaris for subsequent harvesting was investigated using single flocculants of inorganic salts, synthetic polymer, chitosan and dual flocculants of inorganic salts and chitosan. Synthetic polymer (FlopamTM) could achieve over 90% optical density removal (OD680removal) at a low flocculant dose (20 to 40 mg polymer per litre of algal suspension) through the bridging mechanism and charge neutralisation. Inorganic salts (i.e. ferric chloride and aluminium sulphate) and chitosan individually resulted in low flocculation efficiency (<90%) despite high dose (i.e. 160 to 200 mg per litre of algal suspension). The dual flocculation combining ferric chloride or aluminium sulphate with chitosan induced synergistic effects, resulting in >80% flocculation efficiency, significantly higher than the sum of each individual flocculation. The improvement in flocculation efficiency was 57 and 24% respectively for ferric chloride/chitosan and aluminium sulphate/chitosan. Charge neutralisation of microalgal cells by ferric chloride or aluminium sulphate combined with bridging by chitosan produced the synergy.