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The growth of γ-In2Se3 thin films on mica by molecular beam epitaxy is studied. Single-crystalline γ-In2Se3 is achieved at a relatively low growth temperature. An ultrathinβ-In2Se3 buffer layer is observed to nucleate and grow through a process of self-organization at initial deposition, which facilitates subsequent monolithic epitaxy of single-crystallineγ-In2Se3 at low temperature. Strong room-temperature photoluminescence and moderate optoelectronic response are ob-served in the achievedγ-In2Se3 thin films.