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Abstract: Si films with <111> preferred orientation have been prepared on 6H–SiC(000−1) C-face. HRTEM and SAED results indicate that the Si film has epitaxial connection with the 6H–SiC substrate and the parallel-plane relationship of the Si/6H–SiC heterostructure is (111)Si//(000−1)6H–SiC. Using fast Fourier transform and Fourier mask filtering technique, misfit dislocations are clearly observed at the Si/6H–SiC interface, which accommodate the most of lattice mismatch strain. Every four Si (111) lattice planes are registered with five 6H–SiC(000−1) lattice planes along the interface. Based on the 4:5 lattice matching mode, the lattice structure of the Si/6H–SiC interface and its stability were energetically investigated by molecular dynamics simulations. When the Si films grow preferentially along <111> orientation on 6H–SiC(000−1) C-face, the misfit strain in Si layer significantly reduces due to the relaxation of C atoms in SiC layer near the Si/6H–SiC interface, and thus the Si/6H–SiC heterostructure has a stable interface with a small interface formation energy of −14.24eV. [Copyright &y& Elsevier]