An extensive redistribution of spin density in TBrPP-Co molecules adsorbed on a Cu(111) surface is investigated by monitoring Kondo resonances at different locations on single molecules. Remarkably, the width of the Kondo resonance is found to be much larger on the organic ligands than on the central cobalt atom-reflecting enhanced spin-electron interactions on molecular orbitals. This unusual effect is explained by means of first-principles and numerical renormalization-group calculations highlighting the possibility to engineer spin polarization by exploiting interfacial charge transfer.