AbstractDownsizing the cell size of honeycomb monoliths to nanoscale would offer high freedom of nanostructure design beyond their capability for broad applications in different fields. However, the microminiaturization of honeycomb monoliths remains a challenge. Here, we report the fabrication of microminiaturized honeycomb monoliths—honeycomb alumina nanoscaffold—and thus as a robust nanostructuring platform to assemble active materials for micro-supercapacitors. The representative honeycomb alumina nanoscaffold with hexagonal cell arrangement and 400 nm inter-cell spacing has an ultrathin but stiff nanoscaffold with only 16 ± 2 nm cell-wall-thickness, resulting in a cell density of 4.65 × 10⁹ cells per square inch, a surface area enhancement factor of 240, and a relative density of 0.0784. These features allow nanoelectrodes based on honeycomb alumina nanoscaffold synergizing both effective ion migration and ample electroactive surface area within limited footprint. A micro-supercapacitor is finally constructed and exhibits record high performance, suggesting the feasibility of the current design for energy storage devices.