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Abstract: A novel method was proposed for successful fabrication of CuS nanostructures with various morphologies. At the ionic liquids (ILs)-modulated CHCl3–H2O interface, copper cupferronate [Cu(cup)2] in CHCl3 reacted with thiourea in water to generate CuS nanostructures via a solvothermal reaction process. The effects of alkyl chain length of imidazolium cations and nature of anions of the ILs, molar ratio of Cu(cup)2 to thiourea, the reaction temperature and time on the morphology of the products were studied systematically. It was shown that by changing alkyl chain length of imidazolium cations and nature of anions of the ILs, CuS nanostructures with various morphologies, including flowers, urchins, large nanodisks and nanoparticles, could be obtained at the liquid–liquid interface, and the ILs played important template roles in directing the formation of CuS nanostructures. Furthermore, the as-prepared CuS samples exhibited high catalytic activity for photodegradation of methyl orange and thermal decomposition of ammonium perchlorate. [Copyright &y& Elsevier]