Developing high-performance sorbents for volatile organic compounds (VOCs) is urgently required for environmental cleaning and personnel protection. Zirconium-based metal-organic frameworks (Zr-MOFs) have been deemed attractive candidates for gaseous toluene capture due to their superior stability and high adsorption capacity. However, the practical application of powdered Zr-MOFs is hindered by inherent limitations. Here, we report a series of defective UiO-66 metal-organic gels (G66-X) with variable missing linker deficiency by altering the modulator concentration. The defect concentration of the adsorbents has a significant impact on the porosity and gaseous toluene adsorption capacity. Dynamic breakthrough results reveal that G66-9 demonstrates optimal breakthrough time of 336 min/g and uptake amount of 334 mg/g, outperforming those of many other typical toluene adsorbents. The breakthrough times and the uptake capacities dramatically decrease with the increase of adsorption temperature. An outstanding regeneration performance of adsorbents can almost maintain even after five adsorption-desorption cycles.