Sustainable Microplastic Remediation with Record Capacity Unleashed via Surface Engineering of Natural Fungal Mycelium Framework

Plastic‐induced pollution has recently triggered global environmental, biodiversity, and public health concerns. Plastic micro/nanoparticles suspended in water that are non‐recyclable and non‐degradable are found in plants, animals, and even human blood, and their remediation represents an emergent societal need. In this study, a highly efficient strategy is reported to remove microplastics by using a sustainable framework derived from fungal mycelium (FM), which has reached a record capacity at 2.49 g g−1, as it is known. This excellent removal capacity results from both the inherent properties and surface cationization of the FM. First, FM has a loose entanglement and porous structure with extracellular polymeric substances on the surface, which endows FM with the capacity to adsorb microplastics. Second, FM is engineered with 2,3‐epoxypropyltrimethylammonium chloride (EPTAC) to enable its positively charged surface, which significantly enhances the adsorption of microplastics. Kinetic analysis and density functional theory reveal that the excellent microplastic removal is attributed to the enhanced electrostatic interaction between microplastics and EPTAC‐g‐FM. Along with the inherent merits of FM, which are natural, renewable, biodegradable, environmentally friendly, and easy to scale up, FM represents a green, facile, and cost‐effective next‐generation technology for remediating microplastics in clean water. Renewable, biodegradable, scalable, and cost‐effective clean water technology for microplastic remediation is developed from natural fungal mycelium through surface charge engineering, which enables record removal efficiency.