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A method is introduced to correlate electromagnetic theory and polarimetric experiments for anisotropic optically active crystals at oblique angles of incidence. It is based on the 4 × 4 algebraic descriptions of light propagation in layered anisotropic media, which can be simplified to 2 × 2 matrices when multiple reflections are disregarded. Spectroscopic Mueller matrix measurements in transmission and at oblique angles of incidence have been made on two uniaxial crystals: α-quartz and silver thiogallate. Their optical activity tensors have been spectroscopically determined using the method presented here.