Potassium dihydrogen phosphate (KDP) crystals are widely used in laser ignition facilities as optical switching and frequency conversion components. These crystals are soft, brittle, and sensitive to external conditions (e.g., humidity, temperature, and applied stress). Hence, conventional characterization methods, such as transmission electron microscopy, cannot be used to study the mechanisms of material deformation. Nevertheless, understanding the mechanism of plastic-brittle transition in KDP crystals is important to prevent the fracture damage during the machining process. This study explores the plastic deformation and brittle fracture mechanisms of KDP crystals through nanoindentation experiments and theoretical calculations. The results show that dislocation nucleation and propagation are the main mechanisms of plastic deformation in KDP crystals, and dislocation pileup leads to brittle fracture during nanoindentation. Nanoindentation experiments using various indenters indicate that the external stress fields influence the plastic deformation of KDP crystals, and plastic deformation and brittle fracture are related to the material's anisotropy. However, the effect of loading rate on the KDP crystal deformation is practically negligible. The results of this research provide important information on reducing machining-induced damage and further improving the optical performance of KDP crystal components.