Transition metal layered double hydroxide (LDH) nanomaterials have gained wide attention in the fields of supercapacitors, photocatalysis, and electrocatalysis due to their large specific surface area and eminent catalytic performance. In this work, hierarchical NiMn LDH nanosheet arrays were synthesized on flexible carbon cloth (CC) through a one-step hydrothermal reaction as a self-supporting electrode. For one thing, CC can efficiently prevent the aggregation of the NiMn LDH nanosheet and accelerate the electron transfer ability as a desired electric conductor. For another, the synthesized NiMn LDH nanostructures exhibited super electrocatalytic activity toward H 2 O 2 oxidation due to the large active surface area and the synergistic effect of Ni and Mn. Therefore, the nanostructured NiMn LDH on CC displays excellent sensing characteristic for H 2 O 2 with a broad linear range of 1−23,000 μM, a low detection limit of 0.26 μM, and a high sensitivity of 4108 μA mM −1 cm −2 . Moreover, the proposed sensor shows promising application prospects for detecting H 2 O 2 in frozen squid and dried tofu, demonstrating its importance in the food industry and food safety.