“…Detection of small molecules such as metabolites, neurotransmitters, and hormones can provide useful biological information for the diagnosis of specific diseases, prediction of treatment responses, and monitoring of health conditions. , Among various sensing techniques, electrochemical detection has great advantages for point-of-care (PoC) applications due to its merits, such as easy miniaturization, low cost, and fast response. , While electroactive small target molecules are easily detected by direct charge transfer from their own redox reactions on electrode surfaces, electrochemically inactive small molecules can also be detected by monitoring the electroactive products generated from highly selective enzymatic reactions with target molecules. , However, electrochemically inactive small molecules, not involving proper enzymatic reactions generating electroactive products, can be detected with affinity-based electrochemical (bio)sensors, in which small target molecules are selectively bound with bioreceptors (e.g., antibodies and aptamers) or biomimetic receptors (e.g., molecularly imprinted polymers). − Traditional affinity-based electrochemical (bio)sensors require either electroactive labels such as labeled secondary antibodies for voltammetric detections or external solutions containing redox probes for electrochemical impedance spectroscopic detections, which are not suitable for PoC applications. , Moreover, the affinity-based (bio)sensors exhibit extremely high binding affinity, which renders highly selective detection of target molecules but creates difficulty in the regeneration of receptors, impeding repetitive and continuous measurements. Therefore, a significant effort has been made on developing “label-free” and “bind-and-read” electrochemical sensing techniques by coimmobilizing (bio)receptors and redox probes on electrode surfaces toward the decentralized on-site monitoring of clinically important molecules. − …”