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To this purpose, we have rationally designed disulfide DNA strands acting as regulators for the assembly or disassembly of the DNA-based structures. Upon reduction these strands loose their regulatory function which causes the system to return to the basal non-assembled resting state. The exploitation of redox chemistry as a new control mechanism will facilitate the implementation of fuelled-DNA self-assembly processes in a synthetic context without the limitations linked to the use of enzymatic reactions. © 2020 WILEY-VCH Verlag GmbH &