Intercalation of $3d$ atoms into layered transition-metal dichalcogenides (TMDs) provides an effective route to tune their magnetism and electronic structure. Using photon-energy-dependent angle-resolved photoemission spectroscopy, we show that Cr intercalation in $2H\text{−}{\mathrm{NbS}}_2$ introduces additional states at the Fermi level ($E_{\mathrm{F}}$) with appreciable $k_z$ dispersion, giving rise to a three-dimensional Fermi surface in contrast to the quasi-two-dimensional character of pristine $2H\text{−}{\mathrm{NbS}}_2$. Combined with first-principles calculations, we demonstrate that this dimensional crossover originates from interlayer hybridization between energetically aligned out-of-plane-oriented orbitals of intercalation and host-layer atoms, leading to a reconstruction of the near-$E_{\mathrm{F}}$ band manifold and enhanced interlayer hopping. Our results establish orbital hybridization as the key microscopic mechanism governing electronic dimensionality and low-energy band reconstruction in intercalated TMDs, and provide a general framework for understanding dimensional crossover in intercalated van der Waals materials.

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• Electronic structure
• Transition metal dichalcogenides
• Angle-resolved photoemission spectroscopy