Crystalline solids are governed by universal structure-property relationships derived from their crystal symmetry, leading to paradigmatic rules on what properties they can and cannot exhibit. A long-held structure-property relationship is that centrosymmetric crystals cannot differentially absorb circularly polarized light. In this study, we demonstrate the design, synthesis, and characterization of the centrosymmetric material Li 2 Co 3 (SeO 3 ) 4 , which violates this relationship not by defying symmetry-imposed selection rules but by invoking a photophysical process not previously characterized for crystalline solids. This process originates from an interference between linear dichroism and linear birefringence, referred to as LD-LB, and involves strong chiroptical signals that invert upon sample flipping. In addition to enabling a chiroptical response under centrosymmetry, this process opens up photonic engineering opportunities based on crystalline solids.