A proton transfer compound (2a4mpH)₂(btcH₂) was obtained by the reaction of benzene-1,2,4,5-tetracarboxylic acid (btcH₄) with 2-amino-4-methyl pyridine (2a4mp), 1:1 mole ratio and is characterized by IR spectroscopy and single crystal X-ray diffraction analysis. The ion pair is crystallized in monoclinic system and P2₁/c space group with following cell parameters: a = 11.321(2) Å, b = 13.553(2) Å, c =7.026(1) Å, β = 102.473(4)° and Z=2. The final R value is 0.0357 for 9407 total reflections. In the crystal structure, strong and weak O–H···O, N–H···O, C–H···O hydrogen bonds as well as C–H∙∙∙π and ionic interactions connect the various components into a self-associated supramolecular structure.