A relationship between molecular structures of three thiosemicarbazone derivatives and their inhibition capability was studied using electrochemical measurements (potentiodynamic polarization and EIS), molecular dynamics method and quantum chemical calculations. Electrochemical measurements results revealed that the inhibition efficiencies increased with the concentration of inhibitors. The molecular dynamic method results showed that the higher binding energy between the inhibitor and metal surface, the higher the adsorption energy and the higher the inhibition efficiency. Thiosemicarbazone derivatives have been simulated as adsorbate on Ni(111) substrate and the adsorption density, adsorption energy and binding energy have been identified on nickel surface.