The adsorption and corrosion inhibition behavior of three selected thiosemicarbazone derivatives, namely 3-pyridinecarboxaldehycle thiosemicarbazone (META), isonicotinaldehyde thiosemicarbazone (PARA) and 2-pyridinecarboxaldehyde thiosemicarbazone (ORTHO) at the nickel surface were studied electrochemically by Tafel and impedance methods and computationally by carrying out Monte Carlo searches of configurational space on nickel/thiosemicarbazone derivative system. Electrochemical measurements showed that the inhibition efficiency of these compounds increased with increase in their concentration. The recorded inhibition efficiencies of the three tested thiosemicarbazone increase in the order: META > PARA > ORTHO. Polarization studies showed that these compounds act as mixed-type inhibitors for nickel corrosion in 1.0 M HNO3 solutions. Results obtained from Tafel and impedance methods are in good agreement. Thiosemicarbazone derivatives have been simulated as adsorbate on Ni (111) substrate and the adsorption energy, binding energy and the low energy adsorption sites have been identified on nickel surface. (C) 2010 Elsevier Ltd. All rights reserved.