Direct alcohol fuel cells are popular due to their high energy density, abundant sources, and ease of transportation and storage. Palladium-based nanosheet self-assembled materials have emerged as an effective catalyst for alcohol oxidation reactions. In this work, nanosheets were synthesized with the same feeding ratio assembly of alloyed PdM (M = Ag, Cu, and Sn). The introduction of the second element was able to enhance the catalytic response of the catalysts to alcohol electrooxidation. Among them, the PdCu alloy exhibited the best performance in terms of catalytic activity, toxicity resistance, and stability to ethanol oxidation reaction (EOR) and methanol oxidation reaction (MOR). The catalytic current densities for EOR can reach 2226, 2518, and 1598 mA mg-1 for PdAg, PdCu, and PdSn nanosheet assemblies, respectively. These are mainly attributed to better electronic effects, altered atomic distances within the cell for the d-band centers of Pd, and a larger electrochemical active surface area (ECSA). The optimized d-band center is beneficial to promote the catalytic performance of EOR and MOR. Experimental data also demonstrated that higher electrocatalytic temperature, higher pH, and higher alcohol concentration can accelerate the rate of alcohol electrooxidation. These results have the potential to be extended to Pd-M (M = other metals) nanosheets and help for a wider range of catalytic applications.