Metals are important parts of bioelectronic techniques, corresponding to contact electrodes, interconnects, and sensors. Nevertheless, their inherent rigidity poses main challenges for integration in gentle bioelectronics. Particularly, the mechanical mismatch between metals and organic tissues could cause lowered sign constancy and undesirable tissue injury. To deal with these points, numerous geometrical engineering approaches have been explored to extend the deformability of metals. For instance, strain-relief layers have been investigated; nevertheless, bodily laminated constructions typically fail to adequately dissipate pressure beneath deformation. Right here, we current a chemically conjugated, monolithic steel–hydrogel bilayer, imparting excessive deformability to metals with minimal compromise in electrical conductivity. The formation of chemically anchored ligand interactions between the steel and hydrogel induces uniform wrinkles within the steel layer, successfully mitigating stress focus. Consequently, the monolithic bilayer displays ultrasoft mechanical properties and metallic electrical efficiency, together with excessive electrical conductivity, low impedance, tissue adhesion, and stretchability. The chemical anchoring course of is spatially programmable, making it appropriate for the fabrication of arrays of sentimental bioelectronic gadgets. We validated the efficiency and performance of this platform in cardiac functions, demonstrating its efficacy in each electrophysiological recording and electrical stimulation.