Owing to their intrinsically high activity and rich active sites on the surface, noble metal materials with an ultrathin two-dimensional nanosheet structure are emerging as ideal catalysts for boosting fuel cell reactions. However, the realization of controllable synthesis of multimetallic Pd-based alloy ultrathin nanosheets (NSs) for achieving enhanced electrocatalysis evolved from compositional and structural advantages remains a grand challenge. Herein, we report a universal method for the construction of a new series of the three-dimensional (3D) multimetallic PdCuM (M = Ru, Rh, Ir) superstructures that consist of ultrathin alloy NSs. Different from the conventional 2D ultrathin nanostructure, the 3D PdCuM NSs that endowed with abundant routes for fast mass transport, high noble material utilization efficiency, and ligand effect from M to PdCu display large promotion in electrocatalytic performance for the methanol oxidation reaction. Impressively, the composition-optimized Pd59Cu33Ru8 NSs, Pd57Cu34Rh9 NSs, and Pd63Cu29Ir8 NSs show the mass activities of 1660.8, 1184.4, and 1554.8 mA mg-1 in alkaline media, which are 4.9, 3.5, and 4.6-fold larger than that of commercial Pd/C, respectively. More importantly, all of the PdCuM NSs are also very stable for long-term electrochemical tests.