Co element was introduced into the In2O3 system to optimize the catalyst of the hydrogenation of CO2 to methanol. Using hydrothermal method, layered double hydroxides (LDHs) [Co2+1-xIn3+x(OH)2]x+[Ax/n]n- were used as precursors to synthesize InxCo1-xOy catalyst with different In/Co molarratios. The catalytic performance of CO2 hydrogenation was systematically tested, and the structure and surface chemical properties were characterized. The influence of LDHs precursors on the structure and the structure-activity relationship of the prepared catalyst were discussed. The results show that the catalyst with LDHs precursors can effectively inhibit the formation of CH4 by-product. Even at low GHSV or high temperature, the CH4 selectivity is still lower than 1%. Catalyst In0.25Co0.75Oy shows the best catalytic performance of CO2 hydrogenation to methanol. Under the reaction conditions of P=5.0 MPa, T=300 ℃, H2∶ CO2=3 ∶ 1, GHSV=9 000 cm3/(gcat·h), a methanol yield of 3.75 mmolCH3OH/(gcat·h) was achieved.