Three South Australian source waters of low, mid and high dissolved organic carbon (DOC) levels were evaluated for coagulation efficiency in terms of natural organic matter (NOM) interaction and floc behaviour. Experiments were conducted using aluminium chlorohydrate (ACH) and aluminium sulphate (alum) at different mixing conditions with continuous monitoring of formation and breakage of flocs using a flow-through optical measurement device known as photometric dispersion analyser (PDA). A positive correlation of floc growth against coagulant dosage was found for ACH based on a limiting growth function. Floc structure was assessed by analysis of PDA derived parameters showing promise for more rapid coagulation condition optimisation than subjective visual criteria. Removal of NOM and growth of flocs are influenced more by the hydrophobicity of the NOM than the choice of coagulant. A higher hydrophobic fraction resulted in slower aggregation of flocs with both coagulants and better removal when using alum at controlled pH. (C) 2011 Elsevier B.V. All rights reserved.