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Diamond has been grown on 6H‐SiC single crystal wafers by microwave plasma assisted chemical vapor deposition with a negative bias pretreatment. A high nucleation density of diamond on the substrate has been achieved. Cross‐sectional transmission electron microscopy was employed to study the interfacial microstructure of diamond on 6H‐SiC. Lattice image observations illustrate that diamond is directly formed on the 6H‐SiC substrate. The possibility of local epitaxial nucleation of diamond on the 6H‐SiC substrate and its crystallography are briefly discussed.