Functionalization of zigzag graphene nanoribbon (ZGNR) segment containing 120 C atoms with pyridine (3NV-ZGNR) defects was investigated on the basis of density-functional theory (DFT) calculations, results show that edge-modified ZGNRs by Sc can adsorb multiple hydrogen molecules in a quasi-molecular fashion, thereby can be a potential candidate for hydrogen storage. The stability of Sc functionalization is dictated by a strong binding energy, suggesting a reduction of clustering of metal atoms over the metal-decorated ZGNR.