The invention discloses a phenyl bistriazole compound, and a preparation method and application thereof, and particularly relates to a 1-[4-(1H-1,2,4-triazole-1-yl)phenyl]-1H-1,2,4-triazole single crystal and a preparation method of 1-[4-(1H-1,2,4-triazole-1-yl)phenyl]-1H-1,2,4-triazole. The organic compound is prepared by heating ethylenediamine, 1H-1,2,4-triazole, potassium carbonate, 1,4-diiodobenzene and cuprous iodide through a one-pot method. The preparation method disclosed by the invention has the characteristics simple process operation, low production cost and less environmental pollution, and is suitable for large-scale industrial production. The 1-[4-(1H-1,2,4-triazole-1-yl)phenyl]-1H-1,2,4-triazole single crystal prepared by the invention can be used in the aspect of photoelectric materials, especially dye and luminescent agents.