Atomically sharp epitaxial growth of Bi 2 Se 3 films is achieved on Si (111) substrate with MBE (Molecular Beam Epitaxy). Two-step growth process is found to be a key to achieve interfacial-layer-free epitaxial Bi 2 Se 3 films on Si substrates. With a single-step high temperature growth, second phase clusters are formed at an early stage. On the other hand, with low temperature growth, the film tends to be disordered even in the absence of a second phase. With a low temperature initial growth followed by a high temperature growth, secondphase-free atomically sharp interface is obtained between Bi 2 Se 3 and Si substrate, as verified 2 by RHEED (Reflection High Energy Electron Diffraction), TEM (Transmission Electron Microscopy) and XRD (X-Ray Diffraction). The lattice constant of Bi 2 Se 3 is observed to relax to its bulk value during the first quintuple layer according to RHEED analysis, implying the absence of strain from the substrate. TEM shows a fully epitaxial structure of Bi 2 Se 3 film down to the first quintuple layer without any second phase or an amorphous layer.