Continuous and rapid synthesis of UiO-67 under mild conditions has been achieved by electrochemical methods for the first time. In the reaction system, a zirconium sheet was utilized as electrodes and a metal source for the assembly of UiO-67. High-crystalline UiO-67 with a regular tetrahedral morphology of around 1 μm was obtained within 1.5 h under the optimized solvent composition, voltage, and temperature conditions. This electrochemical synthetic method of UiO-67 in our work overcomes the shortcomings of high temperature and pressure of a traditional solvothermal method, which proposes new ideas for the large-scale and rapid synthesis of UiO-67. The UiO-67 synthesized by an electrochemical method was prepared as a UiO-67−carbon paste electrode (CPE), which exhibited a linear response to hydroquinone (HQ) in the range of 5−300 μM with a detection limit of 3.6 × 10 −9 M (S/N = 3), for the electrochemical detection of HQ. It was confirmed that UiO-67−CPE possessed excellent reusability and antiinterference ability for the detection of HQ, and its detection ability even did not change after standing for 3 months. We further tried to apply UiO-67−CPE to the practical determination of HQ in tap water and river water samples, and the results proved that the recovery rate is 97.9−104.7% in real samples.