Cu-In metallic hybrid is a promising non-noble catalyst for selective electrochemical CO2 reduction (eCO2R) to CO, but the lack of direct assembly with a gas diffusion electrode (GDE) limits the further development of eCO2R to CO with both high Faradaic efficiency (FE) and high current density. In this study, an in situ electrochemical spontaneous precipitation (ESP) method was applied for the first time to prepare GDE-combined Cu-In electrocatalysts. The optimum Cu-In catalyst consists of a nanoscale "core-shell" structure of polycrystalline CuxO covered by the amorphous In(OH)3 interface. Higher than 90% FE of CO production has been achieved. With the synergy of a GDE flow cell and 1 M KOH catholyte, a current density of ∼200 mA cm-2 was reached at -1.17 V (reversible hydrogen electrode), which enabled a CO yield efficiency record of 3.05 mg min-1(CO2/15 mL min-1 with a 2 cm2 electrode). The ratios between CO and H2 produced can be effectively modulated via fine-tuning ESP conditions demonstrating possibility of generating CO or syngas with tuneable ratios. The present study provides a simple approach for constructing novel catalytic interfaces with dual active centers for eCO2R and other emerging electrochemical catalysis research.