Lateral heterostructures of two-dimensional (2D) materials provide an atomically coherent platform to study interfacial electronic structures. However, the influence of different interfacial bonding regimes on local electronic states remains unclear. Here, we perform a comparative study of three InSe-based lateral heterostructures formed with Au (metal), Sb (semimetal), and ${\mathrm{Sb}}_2{\mathrm{Se}}_3$ (semiconductor). Scanning tunneling microscopy and spectroscopy combined with first-principles calculations reveal distinct interfacial bonding and corresponding electronic reconstructions. In the Au/InSe heterostructure, strong orbital hybridization and charge transfer lead to metallic behavior and a reduced local band gap. The Sb/InSe interface exhibits moderate coupling with spatially separated valence- and conduction-band edges, characteristic of type-II alignment. In contrast, the ${\mathrm{Sb}}_2{\mathrm{Se}}_3/\mathrm{InSe}$ heterostructure shows nearly van der Waals–type bonding and preserves the intrinsic InSe band edges. By comparing charge-density difference, electrostatic potential profiles, and local density of states, we establish a clear correspondence between interfacial bonding character and electronic reconstruction. This study provides a microscopic understanding of how interfacial chemistry governs the electronic properties of 2D lateral heterostructures.

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• Electronic structure
• Layered semiconductors
• Density functional theory
• Scanning tunneling microscopy
• Scanning tunneling spectroscopy