The graphene-diamond heterostructure has stimulated extensive research due to its potential applications in high-performance electronic devices. The fabrication of the graphene-diamond heterostructure by conventional methods often suffers from complex processing steps, weak interfacial adhesion, or low graphene coverage. Here, we present a different route for fabricating the graphene-diamond heterostructure. By utilizing manganese chemical vapor catalysis, in situ formation of carbon ${sp}^2$-on-$s{p}^3$ is successfully achieved. The as-grown graphene exhibits high coverage, relatively uniform thickness, and high electron concentration and moderate electron mobility ($1.28\times {10}^{15}\mathrm{c}{\mathrm{m}}^{-2}$ and $219\mathrm{c}{\mathrm{m}}^2{\mathrm{V}}^{-1}{\mathrm{s}}^{-1}$ at room temperature, respectively). Furthermore, both covalently bonded and van der Waals interfaces are evidenced by high-resolution transmission electron microscopy, and the charge transfer at the interfaces is revealed through density functional theory calculations. This manganese chemical vapor catalysis strategy with a simple one-step process provides a different pathway for all-carbon ${sp}^2$-on-$s{p}^3$ electronic devices, which may promote industrial-scale applications.

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• Chemical kinetics, dynamics & catalysis
• Growth
• Surface & interfacial phenomena
• Carbon-based materials
• Graphene
• Interfaces
• Electron microscopy
• Raman spectroscopy
• X-ray photoelectron spectroscopy