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We grew high quality BiInSe₃ single crystals and developed an exquisite process to prepare these crystals as substrates. Well cleaved BiInSe₃ single crystals with subsequent in-situ thermal treatment can obtain atomically flat surface, which is evidenced by the sharp streaky reflection high energy electron diffraction (RHEED) patterns. By optimizing the growth recipe, we successfully grew high quality Bi₂Se₃ thin films on BiInSe₃ single crystal substrates. Owing to the weak Van der Waals bonding between the interlayers of BiInSe₃ substrates, we can easily transfer the Bi₂Se₃ thin films grown on these substrates. The high quality surface morphology and electrical transport characteristics, together with the transferrable feature all prove that BiInSe₃ could be a promising substrate for TI films growth. Our discovery could pave a new pathway for improving the sample quality of topological insulator thin films.