Materials scientists are currently shifting from purely inorganic, organic and silicon-based materials towards hybrid organic–inorganic materials to develop increasingly complex and powerful electronic devices. In this context, it is undeniable that conductive metal–organic frameworks (MOFs) and bistable coordination polymers (CPs) are carving a niche for themselves in the electronics world. The tunability and processability of these materials alongside the combination of electrical conductivity with porosity or spin transition offers unprecedented technological opportunities for their integration into functional devices. This review aims to summarise the chemical strategies that have guided the design of this type of materials and the identified opportunities for further development. We also examine the strategies to process them as thin films and stress the importance of analysing the effects of nanostructuration on their physical properties that might be crucial for device performance. Finally, we showcase relevant examples of functional devices that have received increasing attention from researchers and highlight the opportunities available for more sophisticated applications that could take full advantage of the combination of electrical conductivity and magnetic bistability.