Among the family of intercalated transition-metal dichalcogenides (TMDs), ${\mathrm{Fe}}_x{\mathrm{NbS}}_2$ is found to possess unique current-induced resistive switching behaviors, tunable antiferromagnetic states, and a commensurate charge order, all of which are tied to a critical Fe doping of $x_c=1/3$. However, the electronic origin of such extreme stoichiometry sensitivities remains unclear. Combining angle-resolved photoemission spectroscopy (ARPES) with density functional theory (DFT) calculations, we identify and characterize a dramatic eV-scale electronic restructuring that occurs across the $x_c$. Moment-carrying Fe $3d_{z^2}$ electrons manifest as narrow bands within 200 meV of the Fermi level, distinct from other transition metal intercalated TMD magnets. These states strongly hybridize with itinerant electrons in the TMD layer and rapidly lose coherence above $x_c$ due to correlation-driven effects. This sudden quasiparticle decoherence collapses the Fe-Nb hybridization, which explicitly suppresses the out-of-plane effective Fe-Fe exchange interaction, driving the transformation of the magnetic ground state from an antiferromagnetic stripe phase to a zigzag phase. These observations resemble the exceptional electronic and magnetic sensitivity of strongly correlated systems, and demonstrate that quantifying orbital-specific hybridization via ARPES offers an alternative pathway to evaluate effective magnetic exchange in metallic magnets, complementing inelastic neutron and resonant x-ray scattering probes.

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• Magnetism
• Strongly correlated systems
• Angle-resolved photoemission spectroscopy