A　newly　synthesized　N-6-arylhydrazone-8-azaadenine　derivatives　(1)　showed　significant　differences　in　NMR　spectra　with　previously　synthesized　analogues,　specifically,　the　hydrogens　of　N-1＇H　and　C-3＇H　in　all　the　titled　compounds　showed　two　groups　of　signals　in　their　H-1-NMR　spectra.　In　order　to　investigate　whether　the　duplication　of　proton　signals　were　related　to　a　mixture　of　conformational　isomers　which　rotated　around　C-N-1＇　bond　or　configurational　isomers　which　resulted　from　proton　migration,　variable　temperature　NMR　and　2D-NOESY　experiments　were　carried　out　in　conjunction　with　density　function　theory　(DFT)　calculations　at　the　B3LYP/6-311G　(d,p)//B3LYP/6-31G　(d,p)　level.　The　results　indicated　that　it　was　the　conformational　isomerism　rather　than　hydrogen　transfer　that　induced　the　reproduction　of　proton　signals,　which　was　attributed　to　lower　barrier　energy　and　larger　rate　constant　of　the　former　process.