Self-assembly methods combined with standard top-down approaches are demonstrated to be suitable for fabricating three-dimensional ultracompact hybrid organic/inorganic electronic devices based on rolled-up nanomembranes. Capacitors that are self-wound and manufactured in parallel are almost 2 orders of magnitude smaller than their planar counterparts and exhibit capacitances per footprint area of around 200 μF/cm2. This value significantly exceeds that which was previously reported for metal−insulator−metal capacitors based on Al2O3, and the obtained specific energy (0.55 Wh/kg) would allow their usage as ultracompact supercapacitors. By incorporating organic monolayers into the inorganic nanomembrane structure we can precisely control the electronic characteristics of the devices. The adaptation of the process for creating ultracompact batteries, coils and transformers is an attractive opportunity for reducing the size of energy storage elements, filters, and signal converters. These devices can be employed as implantable electronic circuits or new approaches for energy-harvesting applications. Furthermore, the incorporation of functional organic molecules gives rise to novel devices with almost limitless chemical and biological functionalities.