Mode-I fracture toughness (KIC) and tensile strength (σt) are significant parameters in hydraulic fracturing. Owing to the unique mineral composition and sedimentary environment of shale, the mechanical properties of shale exhibit anisotropy. In this study, the notched semi-circular bend (NSCB) and Brazilian disc (BD) tests were combined with acoustic emission (AE) and digital image correlation (DIC) technology to investigate the anisotropic fracture and tensile behaviors of layered shale. The critical plane approach (CPA) criterion is extended and validated, and the universality of the extended CPA criterion is confirmed for both KIC and σt prediction. In addition, the variation of KIC and σt versus loading angle, the relationship between KIC and σt, the typical failure modes of both NSCB and BD specimens, and the fracture initiation angle of layered shales are discussed comprehensively. The following conclusions were drawn: (1) KIC and σt increased with increasing in the loading angle (β), which indicated significant anisotropy of layered shale, and the AE responses for different loading angles also differed significantly. (2) The variation of anisotropic KIC and σt of different shales could be predicted by adjusting the spatial distribution parameter (Ω0), so that the extended CPA criterion could predict KIC and σt of different shales accurately, which confirmed the universality of the extended CPA criterion for both KIC and σt prediction. (3) There exists an approximately linear or power relationship between KIC and σt, and the power relationship can match both experimental and theoretical results much better. (4) The data from DIC and failure modes confirmed that when β was low, the failure modes were primarily affected by the bedding plane. In contrast, when β was great, the failure modes were primarily affected by the matrix. The NSCB specimens exhibited tensile failure, whereas the BD specimens exhibited more complex failure modes, which were a combination of tensile and shear failure. The results of this study can be used for guiding the design and construction of hydraulic fracturing and rock engineering.