The efficacies and toxicities of chiral drug enantiomers are often dissimilar, necessitating chiral recognition methods. Herein, a polylysine–phenylalanine complex framework was used to prepare molecularly imprinted polymers (MIPs) as sensors with enhanced specific recognition capabilities for levo-lansoprazole. The properties of the MIP sensor were investigated using Fourier-transform infrared spectroscopy and electrochemical methods. The optimal sensor performance was achieved by applying self-assembly times of 30.0 and 25.0 min for the complex framework and levo-lansoprazole, respectively, eight electropolymerization cycles witho-phenylenediamine as the functional monomer, an elution time of 5.0 min using an ethanol/acetic acid/H2O mixture (2/3/8,V/V/V) as the eluent, and a rebound time of 10.0 min. A linear relationship was observed between the sensor response intensity (ΔI) and logarithm of the levo-lansoprazole concentration (l-gC) in the range of 1.0 × 10−13–3.0 × 10−11mol/L. Compared with a conventional MIP sensor, the proposed sensor showed more efficient enantiomeric recognition, with high selectivity and specificity for levo-lansoprazole. The sensor was successfully applied to levo-lansoprazole detection in enteric-coated lansoprazole tablets, thus demonstrating its suitability for practical applications.