Biofouling is one of the most critical issues that jeopardizes membrane separation performance, accounting for nearly half of all types of membrane fouling. Herein, inspired by the actions of cuttlefish, we propose an effective strategy to mitigate fouling by fabricating a zwitterionic polymer-brush-modified graphene oxide tethered with trimethylamine-N-oxide (TMAO) head groups. Following a facile vacuum filtration approach with in situ crosslinking, the corresponding 2D membranes (T-GO) were constructed with tunable surface thicknesses and reasonable mechanical robustness. Owing to its unique transport pathways, an optimal membrane exhibits a typical characteristic of nanofiltration with excellent water permeability and a considerably high “solute–solute” selectivity of 18.6 ± 0.3 (toward Congo red/Na₂SO₄), demonstrating a great potential for desalinating textile wastewaters. As the positively and negatively charged head groups are directly connected via a single covalent N–O bond, the O atom can accept three hydrogen bonds in a single polymeric chain, as revealed by the first-principles molecular dynamics simulations. The robust surface hydration layer, induced by surface hydrophilicity, and the disinfection effect, brought by the quaternary ammonium groups, both contribute to the remarkable antiadhesion and contact inactivation ability of the T-GO membrane. Therefore, the antibacterial properties of the T-GO membrane were significantly enhanced, which was experimentally verified for the first time in both the static contact mode and dynamic microfluidic operations. In general, our results provide a robust methodology for designing a new class of nonfouling zwitterionic membranes for sustainable membrane applications.

生物污染是危害膜分离性能的最关键问题之一，占所有类型膜污染的近一半。在此，受墨鱼行为的启发，我们提出了一种有效的策略，通过制造与三甲胺-N-氧化物（TMAO）头基相连的两性离子聚合物刷改性氧化石墨烯来减轻结垢。遵循简单的真空过滤方法，原位交联后，相应的二维膜 (T-GO) 具有可调的表面厚度和合理的机械强度。由于其独特的传输途径，最佳膜表现出纳滤的典型特征，具有优异的透水性和相当高的“溶质-溶质”选择性，为 18.6 ± 0.3（对刚果红/Na ₂ SO ₄)，展示了纺织废水脱盐的巨大潜力。由于带正电荷和带负电荷的头部基团通过单个共价 N-O 键直接连接，如第一性原理分子动力学模拟所示，O 原子可以在单个聚合物链中接受三个氢键。由表面亲水性引起的坚固的表面水化层和由季铵基团带来的消毒作用，都有助于 T-GO 膜具有显着的抗粘附和接触灭活能力。因此，T-GO膜的抗菌性能显着增强，这在静态接触模式和动态微流体操作中首次得到实验验证。一般来说，