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Despite a growing interest in DNA nanomaterials, their simple synthesis remains a challenge. A simple and general strategy for constructing DNA-based nanomaterials by metal ion coordination is reported. The metal-DNA nanoparticles(NPs) could be synthesized with DNA molecules of diverse sequence and various metal ions of intrinsic property, resulting in multifunctional NPs with the combined advantages of both inorganic and DNA building blocks. It is demonstrated that the hybrid metal-DNA NPs could be engineered for magnetic resonance and luminescence imaging, encapsulation of multifarious nucleic acids with controlled ratio, and co-assembly with small drug molecules. Furthermore, because these metal-DNA NPs exhibited enhanced cellular uptake compared to free synthetic DNA, they hold potential for applications in diagnostics and therapeutics.