In view of the environmental pollution caused by the widespread use of reactive dyes in the printing and dyeing industry, the modified cotton fabric was loaded with the extremely stable metal-organic frame (MOF) material UiO-66 for removing reactive dyes from colored wastewater. UiO-66/cotton fabric was prepared by in situ synthesis, and its surface morphology and structure were analyzed by XRD, SEM, BET, and XPS. The adsorption performance of UiO-66/cotton fabric on reactive dyes was investigated by adsorbent dosage, adsorption time and temperature, dye concentration, pH, and so on. The results indicated that the adsorption equilibrium time of UiO-66/cotton fabric on reactive orange 16 was 120 min, and the removal rate was about 98%. The adsorption process belongs to simple molecular layer chemisorption and can be regarded as a spontaneous heat absorption reaction, which was consistent with the proposed secondary kinetic model and Langmuir isothermal adsorption model. In addition, the reactive dyes with a higher molecular weight of each sulfonic acid group are more hydrophobic, and the dyes are more likely to aggregate and deposit on the adsorbent surface by electrostatic attraction, hydrogen bonding, and π-π accumulation. Therefore, this work provides a potential UiO-66/cotton fabric application for the effective adsorption of reactive dyes in textile wastewater.