Graphene hydrogels hold great potential for the disinfection of bacteria-contaminated water. However, the intrinsic antibacterial activity of graphene hydrogels is not satisfactory, and the incorporation of other antibacterial agents often results in their unwanted releases. Here, we present a new strategy to improve the antibacterial activities of graphene hydrogels. We first synthesized a new pi-conjugated molecule containing five aromatic rings and two side-linked quaternary ammonium (QA) groups, denoted as piQA. Next, we fabricated composite gravity filters by assembling piQA with reduced graphene oxide (rGO) hydrogel. The rGO hydrogel helps to form a sponge-like physical sieve, contributes to the overall antibacterial activity, and provides abundant pi-rich surfaces. The large aromatic cores of piQA allow the formation of collectively strong pi-pi interactions with rGO, resulting in a high piQA mass loading of similar to 31 wt%. Due to the sieving effect of rGO hydrogel and the synergistic antibacterial activity of rGO and piQA, the filters prepared based on piQA-rGO assemblies can remove over 99.5% of Gram-negative Escherichia coli (E. coli) and Gram-positive Staphylococcus aureus (S. aureus) cells with a high-water treatment capacity of 10 L g(-1). Furthermore, the piQA-rGO assemblies show low toxicity towards two different mammalian cell lines (L929 and macrophages), and the release of piQA is also negligible. Overall, the new piQA-rGO assembly demonstrates high potential for water disinfection applications. (C) 2018 Elsevier Inc. All rights reserved.