Slate with inherently transverse isotropy is abundant in metamorphic rock, in buildings, and in geotechnical engineering worldwide; the tensile and shear fracture behavior of layered slate is vital to know for engineering applications. In this paper, the Brazilian and semi-circular bend (SCB) tests of layered slate were performed. The fracture characteristics of the slate were investigated by numerical simulations developed by the hybrid finite and cohesive element method (FCEM). Results showed that the measured experimental tensile strength, and mode I fracture toughness of layered slate all showed a typical V-type trend as the bedding angle increased from 0° to 90°, and with divider type. The developed empirical relationship between tensile fracture toughness and tensile strength K_IC = 0.094σ_t + 0.036 fitted experimentally and strongly correlated. The mechanical response and fracture patterns predicted by FCEM agreed well with those of the laboratory experiments. Moreover, the shear fracture behavior and mode II fracture toughness of the layered slate were explored by systematic numerical simulations. Research results provide potential insights for further prediction and improvement of the complex fracture behavior of anisotropic rock masses for rock engineering.