AbstractMulti‐scale organization of molecular and living components is one of the most critical parameters that regulate charge transport in electroactive systems—whether abiotic, biotic, or hybrid interfaces. In this article, an overview of the current state‐of‐the‐art for controlling molecular order, nanoscale assembly, microstructure domains, and macroscale architectures of electroactive organic interfaces used for biomedical applications is provided. Discussed herein are the leading strategies and challenges to date for engineering the multi‐scale organization of electroactive organic materials, including biomolecule‐based materials, synthetic conjugated molecules, polymers, and their biohybrid analogs. Importantly, this review provides a unique discussion on how the dependence of conduction phenomena on structural organization is observed for electroactive organic materials, as well as for their living counterparts in electrogenic tissues and biotic‐abiotic interfaces. Expansion of fabrication capabilities that enable higher resolution and throughput for the engineering of ordered, patterned, and architecture electroactive systems will significantly impact the future of bioelectronic technologies for medical devices, bioinspired harvesting platforms, and in vitro models of electroactive tissues. In summary, this article presents how ordering at multiple scales is important for modulating transport in both the electroactive organic, abiotic, and living components of bioelectronic systems.