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To study the effects of the anisotropic matrix and structural planes on the splitting strength and failure mode of rocks, Brazilian splitting tests were carried out with seven different loading angles on specimens of rock-like materials with rough structural planes. The surface strains of the samples during the failure process were monitored and analysed with the help of a high-speed camera and digital image correlation (DIC) technology. The test results showed that the Brazilian splitting strength (BSS) decreased gradually with an increased loading angle. According to the crack morphology, the samples showed three failure modes, and the structural plane and the loading angle (θ) had an important effect on the failure mode. When θ < 75°, the sample failure was mainly affected by the matrix, and when θ > 75°, the sample failure was mainly controlled by the structural plane. The numerical simulation of the sample with a structural plane was carried out by the PFC2D particle flow program, the micro parameters were calibrated using a back propagation (BP) neural network model. The internal cracks of the sample under a splitting load were mainly matrix tensile microcracks and structural plane shear microcracks, and the tensile microcracks in the side with the weak matrix appeared significantly earlier than those in the side with the strong matrix. With increasing loading angle, the proportion of tensile microcracks in the matrix increased, while the proportion of shear microcracks in the matrix decreased, especially in the weak matrix. The microcracks at the structural plane mainly changed from tensile microcracks to shear microcracks, and the development degree of microcracks along the structural plane was more significant than that on the weak matrix with increasing loading angle. The results of the study can provide a reference for rock stability evaluation and utilization. [ABSTRACT FROM AUTHOR]