† Electronic supplementary information (ESI) available: Maldi-ToF spectrum of [TbPc2] 0 (Fig. S1). UV/vis/nIR spectrum of [TbPc2] 0 (Fig. S2). MOKE spectrum of a blank Si substrate (Fig. S3). VASE spectra of one sample and the model fit (Fig. S4), and in-plane components (Fig. S5), as well as the out-of-plane components of the dielectric tensor (Fig. S6) of the TbPc2 films grown on SiO2/Si. Complex refractive index of TbPc2/PTCDA (Fig. S7). Complex refractive index of TbPc2/Co (Fig. S8). Ligand field parameters of TbPc2 powder and film (Table S1).In this work, we investigated the magneto-optical response of thin films of TbPc2 on substrates which are relevant for (spin) organic field effect transistors (SiO2) or vertical spin valves (Co) in order to explore the possibility of implementing TbPc2 in magneto-electronic devices, the functionality of which includes optical reading. The optical and magneto-optical properties of TbPc2 thin films prepared by organic molecular beam deposition (OMBD) on silicon substrates covered with native oxide were investigated by variable angle spectroscopic ellipsometry (VASE) and magneto-optical Kerr effect (MOKE) spectroscopy at room temperature. The magneto-optical activity of the TbPc2 films can be significantly enhanced by one to two orders of magnitude when changing the molecular orientation (from nearly standing molecules on SiO2/Si substrates to nearly lying molecules on perylene-3,4,9,10-tetracarboxylic dianhydride (PTCDA) templated SiO2/Si substrates) or by using metallic ferromagnetic substrates (Co).