Charge transport through discrete magnetic molecules allows us to exploit quantized molecular charge and spin states, resulting in non-trivial and, from a technology point of view, highly promising charge transport phenomena. However, the integration of single molecules into nanoelectronic environments requires us to establish precisely defined contact modes between single molecules and both conducting (metallic) and non-conducting (oxide) interfaces, which thus far has not been achieved in a reproducible manner. Creating molecular contact modes with exactly defined geometries thus remains a central challenge in molecular electronics. Furthermore, the study of such single-molecule devices also requires a comprehensive understanding of how such molecule/surface contacts affect the molecular electronic and magnetic characteristics. If we want to systematically address both of these issues, we require tractable molecular model systems. As illustrated in this presentation, an ideal class of materials in this context are polyoxometalates, i.e. molecular metal oxide polyanions of the early transition metals V, Mo, W etc. [1] which self-assemble to cluster structures matching proteins in size and structural complexity [2]. As will be shown, polyoxometalates can be functionalized to yield suitable model systems mimicking the highly anisotropic charge environments that are representative of those experienced by molecules in devices such as transistors or spin valves. Attaching e.g. molecular magnets to polyoxometalates allows studying the non-trivial effects of the molecule/model surface binding modes and geometries on the molecular magnetism [3], which in turn determines the single-molecule conductivity features. Moreover, magnetically functionalized polyoxometalates also are the starting point for synthesis strategies that allow – for the first time – to attach nanoscopic electrode precursor structures directly to the molecular magnet, thereby enabling gated single-molecule charge transport experiments with atomic precision.