We investigated the effects of basicity, sulfate content, and aluminum hydrolyte species on the ability of polyaluminum chloride (PACl) coagulants to remove F-specific RNA bacteriophages from river water at a pH range of 6-8. An increase in PACl basicity from 1.5 to 2.1 and the absence of sulfate led to a reduction of the amount of monomeric aluminum species (i.e., an increase of the total amount of polymeric aluminum and colloidal aluminum species) in the PACl, to an increase in the colloid charge density of the PACl, or to both and, as a result, to high virus removal efficiency.The efficiency of virus removal at around pH 8 observed with PACl-2.1c, a nonsulfated 2 high-basicity PACl (basicity 2.1-2.2) with a high colloidal aluminum content, was larger than that observed with PACl-2.1b, a nonsulfated high-basicity PACl (basicity 2.1-2.2) with a high polymeric aluminum content. In contrast, although extremely high basicity PACls (e.g., PACl-2.7ns, basicity 2.7) effectively removed turbidity and UV260-absorbing natural organic matter and resulted in a very low residual aluminum concentration, the virus removal ratio with PACl-2.7ns was smaller than the ratio with PACl-2.1c at around pH 8, possibly as a result of a reduction of the colloid charge density of the PACl as the basicity was increased from 2.1 to 2.7. Liquid 27 Al NMR analysis revealed that PACl-2.1c contained Al 30 species, which was not the case for PACl-2.1b or PACl-2.7ns. This result suggests that Al 30 species probably played a major role in virus removal during the coagulation process. In summary, PACl-2.1c, which has high colloidal aluminum content, contains Al 30 species, and has a high colloid charge density, removed viruses more efficiently (>4 log 10 for infectious viruses) than the other aluminum-based coagulants-including commercially available PACls (basicity 1.5-1.8), alum, and PACl-2.7ns-over the entire tested pH (6-8) and coagulant dosage (0.54-5.4 mg-Al/L) ranges.