The electroreforming of ethylene glycol (EG) derived from polyethylene terephthalate (PET) to prepare rewarding chemicals is an ideal solution to solve serious plastic pollution. A wet chemical method is used to synthesize organic-inorganic hybridized PdMn bimetallenes (PdMn O-BMs) catalyst. The PdMn O-BMs catalyst have a rich curled structure of nanosheets. The structural regulation of organic-inorganic hybrid significantly affects the adsorption energy of the reaction intermediates, thus improving the catalytic activity of the catalyst. PdMn O-BMs demonstrated superior performance compared to PdMn bimetallenes in the PET hydrolysate. This unique organic-inorganic hybrid nanostructure can effectively convert PET-derived EG into high-value products, such as glycolic acid (GA) and formate. This research not only unfolds a prospective strategy for the catalysts modified by organic ligand, but also brings about a new opportunity for the transformation of PET derivatives into high-value products.