In this study, zirconium chloride and montmorillonite were used as raw materials to prepare zirconium-loaded montmorillonite by coprecipitation. The effects of modification and adsorption on the surface structure and surface group of zircalmontmorillonite were studied by scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and specific surface area analysis (BET). The adsorption properties of the montmorillonite on sucrose solution were investigated. The results showed that the surface of zirconium loaded montmorillonite was coarser than that of montmorillonite, with a specific surface area of 204.47 m2/g, which was 3.39 times of the former; nano particles accumulation was observed on the surface. FT-IR and XPS results showed that zirconia was successfully loaded on the surface of montmorillonite, and the isoelectric point of zirconia loaded montmorillonite was 7.39. The adsorption test showed that the adsorption capacity of zircalmontmorillonite was 102.54% higher than that of montmorillonite, and the optimum pH and equilibrium time of adsorption on gallic acid from sucrose solution were 7.0 and 300 min, respectively. The adsorption process could be described accurately by the quasi second-stage adsorption kinetic model and Langmuir isotherm adsorption model, and the saturated adsorption capacity reached 129.87 mg/g; the thermodynamic research showed that the adsorption process was endothermic and can proceed spontaneously. After 5 times of regeneration, zirconium loaded montmorillonite can maintain more than 80% of the initial adsorption capacity. Gallic acid was mainly adsorbed by electrostatic attraction and coordination ion exchange of zirconia. In conclusion, zircalmontmorillonite exhibited good adsorption performance for gallic acid in sucrose solution, and it may be a promising adsorbent for sugar engineering.