Molecularly imprinted polymers have been used for the creation of an electrochemical sensor for the detection of sucrose, which are modified by using functionalized graphene (fG). Using AIBN as the free radical initiator and sucrose as the template, imprinted polymers are synthesized. The monomer, 4,4′-diisocyanatodiphenylmethane (DPDI), has both proton donor groups (N-H or O-H) and lone-pair donor groups (C=O). By creating H-bonds with electron donor groups (C=O), the proton donor group in this polymer may interact with the sugar molecule serving as its template. The sensor signals have improved as a result of the interaction between the monomer and the template. Thermogravimetric and differential thermal analysis (TGA/DTA) curves, scanning electron microscopy (SEM), and FT-IR spectroscopy have been employed to characterize the fabricated receptors. The fabricated sensor has exhibited a limit of detection of 16 ppb for the target analyte that is highly sensitive, linear, reversible, regenerative, and selective. Moreover, the sensor’s stability, reproducibility, and reusability have been evaluated for six months, following the device’s manufacturing, and the results revealed similar responses with the percentage error of less than 1%. Most importantly, this sensor has demonstrated a quick response time, which is very sensitive, stable, and selective.