Due to the strong oxidizability of H2O2, rapid, accurate, sensitive, and stable sensors of hydrogen peroxide (H2O2) have attracted wide attention in the chemical industry, food, medicine, household detergents, and environmental monitoring fields. Here, a high-performance H2O2 electrochemical sensing platform is proposed based on an Au nanoparticles@UiO-66 film coated on a carbon cloth (CC) electrode (Au NPs@UiO-66/CC electrode). The Au NPs@UiO-66/CC electrode was prepared through solvothermal growth of a UiO-66 film on a functionalized three-dimensional CC electrode, followed by in situ deposition of Au NPs into the UiO-66 film under a periodic galvanostatic pulse current. The in situ preparation strategy greatly improves the electrical interaction between Au NPs@UiO-66 and the CC substrate without sacrificing the electrochemical activity of the Au NPs@UiO-66/CC electrode. Meanwhile, thanks to the high specific surface area of the three-dimensional Au NPs@UiO-66/CC electrode, the optimized Au NPs@UiO-66/CC electrode illustrates excellent electrochemical detection capability for H2O2 with an extensive linear range (0.1-21 mM), high sensitivity (1048.01 μA mM-1 cm-2), and lower limit of detection [0.033 μM (S/N = 3)] and limit of quantification [0.109 μM (S/N = 3)]. At the same time, the encapsulated structure of Au NPs in the UiO-66 film also endows the composite electrode with specific sensing performance owing to the regular opening channels of the UiO-66 films that prevent large-size interferents from reacting to the electrochemically active Au NPs. Together with all these advantages, the proposed sensing platform would exhibit great potential for electrochemical sensors and bioelectronics.