Flexible, Graphene‐Coated Biocomposite for Highly Sensitive, Real‐Time Molecular Detection

Wearable biosensors hold significant potential for healthcare and environmental applications, and the development of flexible and biocompatible sensing platforms for high accuracy detection of physiological biomarkers remains an elusive goal. Herein, an ultrasensitive, flexible sensor is described that is based on a 3D hierarchical biocomposite comprised of hollow, natural pollen microcapsules that are coated with a conductive graphene layer. Modular assembly of the graphene‐coated microcapsules onto an ultrathin polyethylene terephthalate layer enables a highly flexible sensor configuration with tunable selectivity afforded by subsequent covalent immobilization of antibodies against target antigens. In a proof‐of‐concept example, the biosensor demonstrates ultrahigh sensitivity detection of prostate specific antigen (PSA) down to 1.7 × 10−15m with real‐time feedback and superior performance over conventional 2D graphene‐coated sensors. Importantly, the device performance is consistently high across various bending conditions. Taken together, the results demonstrated in this work highlight the merits of employing lightweight biocomposites as modular building blocks for the design of flexible biosensors with highly responsive and sensitive molecular detection capabilities.