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Our all-solid-state Li||Li cells can operate at very demanding current-capacity conditions of 4 mA/cm 2 -8 mAh/cm 2 . Thousands of hours of continuous cycling are achieved at Coulombic efficiency 99.5% without dendrite formation or side reactions with the electrolyte. © 2020 WILEY-VCH Verlag GmbH Co. KGaA, Weinheim.It is a significant challenge to achieve controllable self-assembly of superstructures for biological applications in living cells. Here, a two-layer core-satellite assembly is driven by a Y-DNA, which is designed