Advanced intelligent wound monitoring is emerging as a critical tool in first-line therapy, supported by innovative products that accelerate the healing process. A novel approach based on molecular imprinting technology was developed to detect biomarkers associated with wound inflammation, using biopolymeric materials. In this study, an electrochemical biosensor for the selective detection of C-reactive protein (CRP) was developed by modifying gold screen-printed electrodes (Au-SPE) with molecularly imprinted polymers (MIPs). The high-performance sensor film was prepared by the electropolymerization of an aniline monomer in the presence of chitosan polysaccharide and a CRP template on the Au-SPE surface. Key parameters, including the removal agent, scanning rate and the number of electropolymerization cycles, were systematically optimized. Optimal MIP performance, characterized by an enhanced electrochemical response upon recognition of the template molecules, was achieved using a scan rate of 50 mV/s and five electropolymerization cycles. The results demonstrated that this biocompatible biosensor platform exhibited exceptional selectivity and sensitivity, enabling the detection of CRP at concentrations ranging from 1 pg/mL to 10 ng/mL. The incorporation of chitosan into the MIP matrix represents a strategic advancement with significant potential for healthcare applications, owing to its inherent biocompatibility and well-documented benefits in tissue engineering. Additionally, chitosan improves the stabilization of macromolecular templates and enhances their binding interactions with functional monomers. Importantly, this study represents one of the first applications of chitosan-based MIPs in point-of-care (PoC) protein diagnostics.