CO2 hydrogenation to methanol is attracting specific interest because of its potential economic and environmental benefits in transforming waste CO2 to value-added hydrocarbons. Copper-based catalysts are documented as efficient and widely applied, whereas insufficient catalytic properties of conventional catalysts hinder their application. Herein, catalysts using Mg-Al hydrotalcite (HT) as the carrier of Cu/ZnO/ZrO2 (CZZ) nanoparticles were prepared to exploit special advantages of hydrotalcite on copper dispersion and catalytic performance. The results show that CZZ nanoparticles can be uniformly dispersed on external surfaces of HT, elevating BET surface areas of CZZ-HT samples by at least 2.5 times compared to pure CZZ. The HT carrier also enriches strong basic sites and hence elevates CO2 adsorption capabilities in the range of reaction temperature. Both copper surface area and copper dispersion of CZZ-HT samples are improved dramatically. A catalyst containing 45.1 wt% of CZZ shows 1.1 times higher copper surface area per gram CZZ and 1.6 times higher copper dispersion than the reference CZZ. Subsequent reactions demonstrate the CZZ-HT samples show remarkably promoted turnover frequency (TOF) for methanol synthesis and retain considerable catalyst stability. The typical catalyst prepared in this research, at the reaction temperature of 523 K and pressure of 3.0 MPa, presents a 68.2% higher methanol STYCu per gram copper and an 117.0% higher SMeOH/SCO ratio than the commercial catalyst. The support HT plays a crucial role for the enhanced catalytic performance physically and chemically. Thus, the as-prepared CZZ-HT catalyst provides a significant improvement for CO2 utilization.