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The structure of complex [PyH][Ni(mnt)2], as determined by X-ray single crystal analysis, consists of pyridinium cations and [Ni(mnt)2]− anions. Crystallographic data for the complex: monoclinic P21/c, a = 16.5430(18) A, b = 6.3847(9) A, c = 17.430(2) A, β = 118.040(7)°, V = 1625.4(3) A3, Z = 4. The [Ni(mnt)2]− anion is not a planar and the CN groups bend away from the S4 plane. The interactions between anions and cations via the formation of bifurcated N–H···N≡C hydrogen bonds give rise to an 1D zigzag chain of alternating cations and anions.