Despite the fact that the majority of charge partition and free energy analyses depict the Ni(II) complex as a viable and cost-effective alternative to Pt for HER, the substantial overpotential of Co(II) underscores the promise of Schiff bases in enhancing Ni(II)'s catalytic efficacy. This interplay between ligand design and catalytic efficiency warrants further investigation to fully capitalize on the potential of Schiff base-modified metal complexes in HER applications.