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Abstract Modern implantable bioelectronics demand soft, biocompatible components that make robust, low‐impedance connections with the body and circuit elements. Concurrently, such technologies must demonstrate high efficiency, with the ability to interface between the body's ionic and external electronic charge carriers. Here, a mixed‐conducting suture, the e‐suture, is presented. Composed of silk, the conducting polymer poly(3,4‐ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS), and insulating jacketing polymers,the resulting e‐suture has mixed‐conducting properties at the interface with biological tissue as well as effective insulation along its length. The e‐suture can be mechanically integrated into electronics, enabling the acquisition of biopotentials such as electrocardiograms, electromyograms, and local field potentials (LFP). Chronic, in vivo acquisition of LFP with e‐sutures remains stable for months with robust brain activity patterns. Furthermore, e‐sutures can establish electrophoretic‐based local drug delivery, potentially offering enhanced anatomical targeting and decreased side effects associated with systemic administration, while maintaining an electrically conducting interface for biopotential monitoring. E‐sutures expand on the conventional role of sutures and wires by providing a soft, biocompatible, and mechanically sound structure that additionally has multifunctional capacity for sensing, stimulation, and drug delivery.