Gadolinium(III) complexes have recently been demonstrated to have potential as polarizing agents for high-field dynamic nuclear polarization (DNP) NMR spectroscopy. By tailoring the ligand design to reduce the zero-field splitting (ZFS), we demonstrate a quadratic improvement in DNP through the investigation of a stable, water-soluble, narrow-line Gd(III) complex, [Gd-(tpatcn)], doubling the magic-angle-spinning DNP enhancement of the previous state-of-the-art [Gd(dota)-(H2O)](-) at 9.4 T and 100 K.