Self-organized nanocrystal architectures with subnanometric spatial resolution were obtained by mimicking the biological crystal growth. The key step of this facile, one-pot, biomimetic route is to induce the self-assembly of the artificial nanopore cucurbit[7]uril with metal ions, which generates supramolecular aggregates that recreate the physicochemical environment of biomineralization processes. The approach holds great promise for the fabrication of nanocrystal superstructures of functional materials, useful in optics, electronics, and catalysis.