ABSTRACT Synthetic 2D materials face persistent bottlenecks in cost, low environmental compatibility, and scale. Meanwhile, owing to their abundant reserves, low cost, environmental compatibility, high cation exchange capacity, and tunable interlayer structure, natural layered vermiculite nanosheets (VMTNSs) have emerged as key alternative materials to mitigate these bottlenecks. This review traces the evolution of VMTNSs research and establishes a methods framework spanning physical, chemical, and physicochemical exfoliation: we compare their mechanisms, process, energy footprints, and scalability. Furthermore, we formalize a structure‐property correlation framework linking stacking number, lateral size, interlayer spacing, and surface functionality to adsorption selectivity, ionic transport, optical/thermal behavior, and biocompatibility. Application case studies demonstrate opportunities in biomedicine (drug delivery, cancer therapy, tissue regeneration and antibacterial), energy (salinity‐gradient conversion, solid‐state electrolytes, sensors), and environment (ion sieving, water/gas treatment) where VMTNSs rival or exceed selected commercial benchmarks. Finally, we identify key challenges in vermiculite nanosheet research‐namely high energy demand, limited stability under complex service conditions, and narrowly scoped functionality. Future work should establish a standardized testing framework that reproduces complex operating conditions and leverage molecular‐dynamics‐guided optimization of composite architectures to achieve precise structure‐property control. This review aims to accelerate the industrial deployment of vermiculite nanosheets, provide a practical reference for materials selection in related fields, and advance carbon‐neutrality targets through sustainable resource utilization.
Ma et al. (Thu,) studied this question.