Nanomaterials that were once considered biologically inert are now found to exhibit some natural enzyme-like catalytic activities. As an emerging generation of artificial enzymes, nanozymes not only have the catalytic activity to accelerate substrate reactions with comparable kinetics of natural enzymes but also maintain good stability under harsh conditions. With these attractive characteristics, extensive applications of nanozymes in various fields have been explored in the past decade. This chapter mainly focuses on the design and applications of nanozymes in the detection of environmental pollutant ions. The detection principles and strategies, including analyte-involved nanozyme reactions, regulating nanozyme activities, and affecting nanozyme catalyzed systems, are discussed in detail. The applications of nanozymes in analyzing typical inorganic ions are summarized and commented on. Moreover, their perspectives and future development trends in this interesting field are also presented.