A heterocyclic phenylhydrazone 2-[(E)-(2-phenylhydrazinylidene)methyl]pyridine (P2APH) and its reduced form 2-[(2-phenylhydrazinyl)methyl]pyridine (RP2APH) were synthesized, characterized, and subjected to corrosion inhibition investigation on carbon steel (CS) in 1 M HCl using gravimetric, polarization, electrochemical noise, quantum chemical, and surface studies. P2APH showed more inhibition capacity than RP2PPH. But RP2PPH was very stable in acid medium and showed pronounced corrosion inhibition efficacy for days. Energy of HOMO and LUMO, their difference, number of electrons transferred, electronegativity, chemical hardness, and so forth were evaluated by quantum chemical studies. Agreeable correlation was observed between the results of quantum chemical calculations and other corrosion monitoring techniques.