Layereddouble hydroxide (LDH) materials have attracted much attentionin electromagnetic (EM) wave absorption applications due to theirflaky texture and adjustable bimetallic composition. However, theconstruction of 2D LDH materials, especially metal-organicframework (MOF)-derived LDHs, is usually demanded with high-energyand multi-step processes. Here, the 2D bimetallic Co, Ni-LM nanosheetshave been readily prepared by a one-step room-temperature reactionusing 2-methylimidazole as an inducer molecule and the interlayerequilibrium substance. The precise molar ratio of Co2+ andNi(2+) in water/methanol is the controlling factor for theformation of MOF-derived LDH nanosheets. In addition, the well-tunedmolar ratio can be extended to the preparation of 2D bimetallic Zn,Ni-LM nanosheets by only changing the Co2+ ions to Zn2+ ions, using the same feeding ratio. Then, we apply a temperature-controlledpyrolysis strategy under air to convert Co, Ni-LM and Zn, Ni-LM intotheir derivatives of Co, Ni-LMc and Zn, Ni-LMc, respectively. Basedon the synergistic effects of multi-components and 2D structure, theCo, Ni-LMc material achieves remarkable electromagnetic absorption(EMA) performance, where its maximum width reaches 4.76 GHz with athickness of 1.9 mm. For Zn, Ni-LMc material, a resonant absorptionpeak appears around 14.04 GHz for different absorber thicknesses.This work enlightens a facile, green, and environmentally friendlystrategy for constructing MOF-derived LDH nanosheets. The unique EMresponse behavior of the two derivatives also provides us with a positiveguidance for the subsequent design of EMA composites to meet the requirementsof different application environments.