The objective of this study was to investigate the removal of the bacteriophage MS2 by Ni/Al layered double hydroxide (LDH). Batch experiments were performed using a powder form of Ni/Al LDH under various conditions. Column experiments were also performed under flow-through conditions with Ni/Al LDH coated sand. Batch tests showed that the powder form of Ni/Al LDH was effective for bacteriophage removal under the given experimental conditions (LDH dose of 2.5 g L(-1); initial MS2 concentration of 1.35 × 10(5) plaque forming unit (pfu) mL(-1)) with a removal capacity of 5.5 × 10(7) pfu g(-1). The results also indicated that the effect of the solution pH on the bacteriophage removal was minimal at pH 4.3-9.4. The influence of divalent anions (SO(2-) (4), CO(2-) (3), HPO(2-) (4); concentrations 1-100 mM) on the removal of the bacteriophage was significant, while the effects of monovalent anions (NO(-) (3), Cl(-)) were negligible. Column experiments showed that the log removal of MS2 was 4.51 in columns containing 100% Ni/Al LDH-coated sand, while it was 0.02 in columns containing 100% quartz sand (initial MS2 concentration of approximately 7.0 × 10(5) pfu mL(-1); flow rate of 0.5 mL min(-1)). These findings indicated that Ni/Al LDH-coated sand was far more effective at removing bacteriophage than sand alone. This study demonstrates that Ni/Al LDH can be used for virus removal in water treatment and filtration applications.