Electrochemical carbon dioxide (CO2) reduction into valuable chemicals is usually implemented at high overpotential, and most bimetallic catalysts suffer from the dramatic evolution of surface composition especially in case of long-term operation. In this work, as a proof-of-concept experiment, one effective protocol is first identified to drive the positive evolution of surface contents on nanoporous Cu-In by electrochemical training in KHCO3 electrolyte. Interestingly, superior performances including high selectivity for CO production and robust reliability are realized. Thus, Faradaic efficiency can approach the maximum of 91% at -0.95 V (vs. RHE), and an excellent durability can be simultaneously testified by no detectable performance decay for 7 h in operation. More importantly, current investigation paves a new road for designing bimetallic electrocatalysts with high selectivity and long-term durability. (C) 2018 Elsevier Ltd. All rights reserved.