Nanozymes have emerged as a class of novel catalytic nanoma-terials that show great potential to substitute natural enzymes in variousapplications. Nevertheless, spatial organization of multiple subunits in ananozyme to rationally engineer its catalytic properties remains to be a grandchallenge. Here, we report a DNA-based approach to encode the organization ofgold nanoparticle clusters (GNCs) for the construction of programmable enzymeequivalents (PEEs). Wefind that single-stranded (ss-) DNA scaffolds can self-fold into nanostructures with prescribed poly-adenine (polyA) loops and double-stranded stems and that the polyA loops serve as specific sites for seed-freenucleation and growth of GNCs with well-defined particle numbers andinterparticle spaces. A spectrum of GNCs, ranging from oligomers with discreteparticle numbers (2-4) to polymer-like chains, are in situ synthesized in thismanner. The polymeric GNCs with multiple spatially organized nanoparticles as subunits show programmable peroxidase-like catalytic activity that can be tuned by the scaffold size and the inter-polyA spacerlength. This study thus opens new routes to the rational design of nanozymes for various biological and biomedical applications.
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