Magnetic molecules are potential functional units for molecular and supramolecular spintronic devices. However, their magnetic and electronic properties depend critically on their interaction with metallic electrodes. Charge transfer and hybridization modify the electronic structure and thereby influence or even quench the molecular magnetic moment. Yet, detection and manipulation of the molecular spin state by means of charge transport, that is, spintronic functionality, mandates a certain level of hybridization of the magnetic orbitals with electrode states. Here we show how a judicious choice of the molecular spin centres determines these critical molecule-electrode contact characteristics. In contrast to late lanthanide analogues, the 4f-orbitals of single bis(phthalocyaninato)-neodymium(III) molecules adsorbed on Cu(100) can be directly accessed by scanning tunnelling microscopy. Hence, they contribute to charge transport, whereas their magnetic moment is sustained as evident from comparing spectroscopic data with ab initio calculations. Our results showcase how tailoring molecular orbitals can yield all-electrically controlled spintronic device concepts.