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An effective approach to enhance the thermoelectric performance (ZT) of polycrystalline In4Se3 based samples by crystallographic and microstructural engineering is proposed and demonstrated. Cu intercalation, Br substitution at selenium sites, and incorporation of dispersed hierarchical nanoparticles are discussed. An improved ZT of 1.1 at 723 K is achieved in CuBr2 doped In4Se2.5.