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Electroreduction of carbon dioxide (CO2) to chemicals is a promising route to convert and utilize CO2 under atmospheric conditions. However, the relative poor reaction efficiency seriously hinders the practical applications of this route. In this work, flowerlike In2S3 assembled by nanoflakes was synthesized via ionothermal method and exhibited a high Faradaic efficiency (FE) of 86 % with excellent formate formation rate of 478 μmol h−1 cm−2 in ionic liquid (IL) electrolyte. Flowerlike structure can provide large electrochemically active surface area and enhance mass transfer rate. Additionally, density functional theory (DFT) calculations reveal that the origin of the improved performance can be attributed to the large adsorption energy of CO2* and OCHO* intermediate on the (440) facet which is the main exposed crystal facet of flowerlike In2S3.[f1] [ABSTRACT FROM AUTHOR]