Two new asymmetrical 3-(p-R-phenyl)-4-amino-5-(2-pyridyl)-1,2,4-triazoles (3a, R = CH 3 and 3b, R = OCH 3 ) were synthesized with a yield of 58% and 69%, respectively. The compounds 3a and 3b were characterized with FT-IR, 1 H NMR, ESI-MS spectra, and elemental analysis. Additionally, their molecular and crystal structures were determined by single crystal X-ray analysis.