Herein, the anti-corrosion of carbon steel in 1 M HCl by two newly synthesized pyrazolotriazole derivatives, namely, 6-methyl-1H-pyrazolo[5,1-c][1,2,4]triazole-7-carbonitrile (CPT) and 1-acetyl-6-methyl-1H-pyrazolo[5,1-c][1,2,4]triazole-7-carbothioamide (MPT), was studied using electrochemical, density functional theory (DFT), and molecular dynamics (MD) simulation techniques. The experimental results showed that the concentrations of inhibitors had a significant influence on their inhibition efficiencies. Potentiodynamic polarization curves indicated that the two pyrazolotriazoles were mixed-type inhibitors. DFT calculations were employed to explore the molecular activity, and MD simulations were performed to obtain the interaction energy between the inhibitor molecules and the iron surface. The findings obtained using the theoretical calculation techniques were consistent with those obtained via experiments.