Polyvinylpyrrolidone Oxime (PVPO) was synthesized and studied for mild steel (MS) corrosion inhibition in 1 M H2SO4, at different concentrations and temperatures. The corrosion inhibition efficiency was studied using weight loss method, polarization technique, electrochemical impedance spectroscopy (EIS), scanning electron microscopy (SEM) and quantum chemical calculations. The results from weight loss, potentiodynamic polarization and EIS showed that the inhibition efficiency (I. E.) increased with gradual increments in the inhibitor concentration, and decreased at higher temperatures. The polarization study also revealed that PVPO acted as a mixed type inhibitor, and Langmuir adsorption isotherm fitted well for the adsorption behavior. The highest corrosion efficiency was found to be 88.39%, with a concentration of 1000 ppm, and a temperature of 303 K. The corrosion inhibition mechanism has been further proposed, including the support from the theoretical study. SEM images also verified the MS surface smoothening in PVPO presence, and, hence, it has shown to be a good corrosion inhibitor.