AbstractMagnetoelectrics with ultra-low symmetry and spin-orbit coupling are well known to display a number of remarkable properties including nonreciprocal directional dichroism. As a polar and chiral magnet, Ni₃TeO₆ is predicted to host this effect in three fundamentally different configurations, although only two have been experimentally verified. Inspired by the opportunity to unravel the structure-property relations of such a unique light-matter interaction, we combined magneto-optical spectroscopy and first-principles calculations to reveal nonreciprocity in the toroidal geometry and compared our findings with the chiral configurations. We find that formation of Ni toroidal moments is responsible for the largest effects near 1.1 eV—a tendency that is captured by our microscopic model and computational implementation. At the same time, we demonstrate deterministic control of nonreciprocal directional dichroism in Ni₃TeO₆ across the entire telecom wavelength range. This discovery will accelerate the development of photonics applications that take advantage of unusual symmetry characteristics.