The corrosion inhibition of ampicillin (AMP) and its synergistic combination with halides (KI, KCl and KBr) for the corrosion of mild steel in H2SO4 have been investigated using gravimetric, gasometric, thermometric and infrared (IR) methods. The inhibition efficiencies of AMP for the corrosion of mild steel increased with increase in concentration but decreased with rise in temperature. The adsorption of AMP on the mild steel surface was found to obey the Langmuir adsorption isotherm model. The combination of AMP with the halides (KI, KBr and KCl) enhanced the inhibition efficiency and adsorption behavior of the inhibitor indicating synergism. The inhibition efficiency of AMP increased with increasing concentration and the adsorption of the inhibitor was spontaneous. Physical adsorption mechanism has been proposed from the thermodynamic data obtained. There was a significant correlation between the inhibition efficiency of AMP and some quantum chemical parameters (R-2 = 0.96) using the quantitative structure-activity relationship (QSAR) method. Some quantum chemical parameters and the Mulliken charge densities on the optimized structure of AMP were calculated using the B3LYP/6-31G (d,p) basis set method to provide further insight into the mechanism of the corrosion inhibition process.