The catalytic transfer-hydrogenation of citral is a vital chemical process in food flavoring, fragrance, and pharmaceutical industries, that necessitates a high degree of purity of the product. However, the heterogeneous catalyst that is mainly selective to α,β-unsaturated alcohol at atmospheric pressure is still lacking. Herein, we prepared a series of mesoporous ZrO₂ via a soft-templated inverse micelle method, using different calcination temperatures 250–600 °C. The effect of the calcination temperature on the intrinsic surface properties of the meso-ZrO₂ was revealed by analytical techniques such as N₂ adsorption-desorption isotherms, pXRD (powder X-ray diffraction), TEM (transmission electron microscope), and CO₂/NH₃-TPD (temperature-programmed desorption). The meso-ZrO₂ catalysts were compared in the Meerwein-Ponndorf-Verley (MPV) reduction of citral at atmospheric pressure. The meso-ZrO₂ calcined at 350 °C presented a superior catalytic activity of 71% citral conversion and 100% selectivity to unsaturated alcohol after 10 h, under optimized reaction conditions. The superior activity is ascribed to the enlarged pore volume, increased surface area, and Lewis acidic sites. The calcination temperature has played a significant role in tailoring the surface properties of the meso-ZrO₂, which in turn enhanced the catalytic activity. The meso-ZrO₂ catalyst is recyclable, easily regenerated with simple calcination. The meso-ZrO₂ shows excellent potential for industrial applications.