Herein, we propose the fabrication of polyethyleneimine-functionalized PdOs bimetallene (PdOs@PEI bimetallene) for the alkaline oxygen reduction reaction (ORR) via a wet-chemical method. The PdOs@PEI bimetallene has an ultra-thin and curved nanosheet structure that is conducive to providing more active sites and high conductivity and the bimetallic composition and PEI modification can tailor the electronic structure of PdOs bimetallene, leading to enhanced oxygen adsorption energy. Therefore, the PdOs@PEI bimetallene exhibits superior ORR activity, stability and durability to commercial Pt/C, highlighting the important role of the modified nitrogen-containing polymers in the enhancement of ORR performance.