Biomolecules are central to their extraordinary effectiveness for biological functions in life. These natural nanotools reinforce the rational fabrication of nanomaterials for many applications in fields, such as plasmonics and biomedicine. Scientists have utilized DNA beyond its biological roles for the preparation of a myriad of self-assemblies or metalized materials while there are issues of mutual concern: the self-assemblies of biomolecules have limited practical uses even though they look fantastic. Moreover, the metallization of the self-assemblies into applicable inorganic materials is currently limited by cost and difficulty, as keeping materials into patterns smaller than 100 nm in size. We aimed to develop groundbreaking technology of highly facile preparation of nanometals with direction-following, shape- and size-controlled architectures via regulation of metallic atom crystallization by DNA. This technology unlocks the toolbox full of smart biomolecules for the synthesis of architecture-programmable metallic nanomaterials. Importantly, the technology will solve one of the most fundamental but difficult problems of bottom-up synthesis: how to tailor nanomaterial’s structure with molecular level precision of design. Hereby, unprecedented nanostructures (e.g. asymmetric metallic nanoparticles) can be generated in extremely specific properties, which holds broad appeal for material scientists and nanotechnologists.