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Two mismatch\u2010binding ligands carrying 2,2,6,6\u2010tetramethylpiperidine <jats:italic>N<\/jats:italic>\u2010oxide (TEMPO) and nitronyl nitroxide selectively bind to the predetermined sites on double stranded DNA. By using the two mismatch\u2010binding ligands carrying the organic radicals as the glue for DNA, electron\u2010spin assembly could be successfully synchronized with the hybridization. Periodically and tandemly arranged, two kinds of organic radical molecules at designed positions might be useful for an approach to build up scalable qubits of electron\u2010spin\u2010based quantum computing. 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