Acute myocardial infarction (AMI) is a severe cardiovascular disease characterized by heart muscle damage due to inadequate blood supply, leading to a life-threatening risk of heart attack. Herein, we report on the design of polyaminophenol-based thin film functional polymers and their thorough optimization by electrochemical, spectroscopic, and microscopic techniques to develop a high-performance pointof-care voltammetric monitoring system. Molecularly imprinted polymerbased cTnI-responsive nanocomposite materials were prepared on an electrode surface by imprinting a specific cTnI epitope, integrating polyaminophenol electrodeposition, along with gold nanoparticles (AuNPs) and graphene quantum dots (GQDs). The characterization techniques, including cyclic and square wave voltammetries, electrochemical impedance spectroscopy, atomic force microscopy, fluorescence microscopy, attenuated total reflection-Fourier transform infrared spectroscopy (ATR-FTIR), and contact angle measurements proved the efficient fabrication of the voltammetric monitoring system relying on cTnI-responsive functional thin films. The sensing platform prepared with the optimized nanocomposite composition of AuNPs, GQDs, and molecularly imprinted polymers exhibited very high sensitivity, reproducibility, specificity, and affinity toward cTnI. The sensor showed a storage stability of 30 days, demonstrating great potential for use in early and point-of-care diagnosis of AMI with its 18 min detection time.