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The reduction of carbon dioxide to valuable chemical products is a hot topic of current research. In this article, Cu nanoparticle-decorated Fe 3 O 4 (Cu/Fe 3 O 4 ) is prepared by using layered double hydroxide (LDH) as the precursor. The CuFe-LDH is synthesized using the coprecipitation method and further reduced to obtain the final material Cu/Fe 3 O 4 . The uniform layered structure of LDH results in highly dispersed metallic elements in the corresponding Cu/Fe 3 O 4 , in which Cu atoms provide Cu 0 and Cu + pairs and good electrical conductivity during the reduction process with Fe 3 O 4 as the framework. Therefore, Cu/Fe 3 O 4 shows high selectivity for CO 2 electroreduction to ethanol, in which the Faraday efficiency is 50.9% at −0.3 V vs RHE. Experimental results show that Cu/Fe 3 O 4 generates uniformly distributed Cu + sites during CO 2 electroreduction, which is conducive to the formation of *CHO, a key intermediate to ethanol. This study provides a design method for catalysts of CO 2 electroreduction with feasibility.