Two new imidazole salts, namely, [HIMT]+ X (X = NO3–) (1), ClO4– (2) [IMT = 4-((1H-imidazol-1-yl)methyl)benzonitrile], were grown through reacting IMT and two different inorganic acids by slow evaporation method, respectively. Salts 1 and 2 have been characterized by single–crystal X–ray diffraction, IR, UV–vis, and thermogravimetric analyses (TGA). In both compounds, a variety of hydrogen bonds (C/N–H⋯O/N) can be obviously obtained, through which a three-dimensional framework will be constructed. The luminescent spectra show that the emission maxima in salts 1 and 2 are observed at 391 and 414 nm, respectively. Compared to the free IMT, the emission bands of its salts 1 and 2 are obviously red-shifted about 49 and 72 nm, respectively.