The chiral helimagnet Cr 1/3 NbS 2 hosts exotic spin textures, whose influence on the magnetotransport properties make this material an ideal candidate for future spintronic applications. To date, the interplay between macroscopic magnetic and transport degrees of freedom is believed to result from a reduction in carrier scattering following spin order. Here, we present electronic structure measurements across the helimagnetic transition temperature T C that challenges this view. We show that the Fermi surface is comprised of strongly hybridized Nband Cr-derived electronic states, and that spectral weight close to the Fermi level increases anomalously as the temperature is lowered below T C. These findings are rationalized on the basis of first principle density functional theory calculations, which reveal a large nearestneighbor exchange energy, suggesting the interaction between local spin moments and hybridized Nb-and Cr-derived itinerant states to go beyond the perturbative interaction of Ruderman-Kittel-Kasuya-Yosida, suggesting instead a mechanism rooted in a Hund's exchange interaction.