Strength anisotropy is one of the most distinct features of anisotropic rocks, and it also normally reveals strong anisotropy in Brazilian test Strength (“BtS”). Theoretical research on the “BtS” of anisotropic rocks is seldom performed, and in particular some significant factors, such as the anisotropic tensile strength of anisotropic rocks, the initial Brazilian disc fracture points, and the stress distribution on the Brazilian disc, are often ignored. The aim of the present paper is to review the state of the art in the experimental studies on the “BtS” of anisotropic rocks since the pioneering work was introduced in 1964, and to propose a novel theoretical method to underpin the failure mechanisms and predict the “BtS” of anisotropic rocks under Brazilian test conditions. The experimental data of Longmaxi Shale-I and Jixi Coal were utilized to verify the proposed method. The results show the predicted “BtS” results show strong agreement with experimental data, the maximum error is only ~6.55% for Longmaxi Shale-I and ~7.50% for Jixi Coal, and the simulated failure patterns of the Longmaxi Shale-I are also consistent with the test results. For the Longmaxi Shale-I, the Brazilian disc experiences tensile failure of the intact rock when 0° ≤ β_w ≤ 24°, shear failure along the weakness planes when 24° ≤ β_w ≤ 76°, and tensile failure along the weakness planes when 76° ≤ β_w ≤ 90°. For the Jixi Coal, the Brazilian disc experiences tensile failure when 0° ≤ β_w ≤ 23° or 76° ≤ β_w ≤ 90°, shear failure along the butt cleats when 23° ≤ β_w ≤ 32°, and shear failure along the face cleats when 32° ≤ β_w ≤ 76°. The proposed method can not only be used to predict the “BtS” and underpin the failure mechanisms of anisotropic rocks containing a single group of weakness planes, but can also be generalized for fractured rocks containing multi-groups of weakness planes.