“…The development of advanced biomolecular electronic interfaces and the elucidation of intricate biomolecular interactions is one of the important approaches for the innovation of new sensing and detection methodologies. , Thereinto, it is critical to rationally construct the interface molecules to seamlessly bridge the synthetic-living interface with conductivity, specificity, and biocompatibility. , Leveraging the inherent properties, peptides are ideal molecular building blocks for achieving the above trifecta through related biosensors and bioelectronics . On one hand, peptides enable artificial controlled molecular synthesis and hybridization as well as ordered morphological self-assembly, making them predictable electronic functions for sensitive sensing. , On the other hand, natural-amino-acid-compounded peptides provide a platform for precise interactions with biological entities, making them promising candidates for recognition and selective measurement. − In recent years, several active-peptide-based bioelectronic interface molecules were reported for electrochemical sensing, which were mainly concentrated on the biomimetic designs of natural-protein deserved peptide segments to facilitate electron transfer through enzymatic-like reactions, biological redox-mediated processes (such as cytochromes), , ion-channels protein fragments (such as gramicidin), , and other mechanisms. , …”