Organophosphorus pesticides are the most extensively utilized agrichemicals in the world. They play a crucial role in regulating crop growth, immunizing against pests, and improving yields, while their unregulated residues exert serious detrimental effects on both the environment and human health. Many efforts have been made in the world to monitor organophosphorus pesticides and solve the issues caused by them. Nanozymes, as one kind of enzyme mimic that is artificially designed to simulate the function of natural enzymes, have aroused a lot of attention due to their unparalleled advantages. Nanozymes inherit both the unique properties of nanomaterials and catalytic functions, which could overcome the limitations inherent in natural enzymes and have great versatile and adaptable application prospects. This review presents a recent advancement in synthesizing multifunctional nanozymes with enzymatic-like activities by using various nanomaterials to degrade and detect organophosphorus pesticides. It mainly encompasses metal-based nanozymes, carbon-based nanozymes, metal-organic-framework-based nanozymes, and single-atom-based nanozymes. Additionally, this paper discusses the potential of nanozymes as novel functional environmental materials.