Molecule-based ferromagnets that exhibit strong second-harmonic generation (SHG) are presented here for the first time. The strategy for producing such materials-replace the ''innocent'' bulky cations (C) in the C[M'M(ox)(3)] family of bimetallic magnets (M' is e.g. Mn and M = Cr-III or Fe-III: the Figure shows the structure) by hyperpolarizable cationic chromophores-is described and X-ray, magnetic, and SHG results are reported.