Two crystalline organic acid-base adducts [(L)Á (Chda), L = 2-aminopyrimidine, Chda = 1,4-cyclohexanedi carboxylic acid] (1), and (2-aminopyrimidine):(butane-1,2,3,4-tetracarboxylic acid):2H 2 O [(HL 1 ) 2 Á(Bta 2-)Á2H 2 O, Bta 2-= dihydrogen butane-1,2,3,4-tetracarboxylate] derived from 2-aminopyrimidine and carboxylic acids (1,4-cyclohexanedicarboxylic acid, and butane-1,2,3,4-tetracarboxylic acid) were prepared and characterized by X-ray diffraction analysis, IR, mp, and elemental analysis. Compound 1 crystallizes in the monoclinic, space group P2(1), with a = 5.2153 (5) Å , b = 18.2803(17) Å , c = 7.3409(6) Å , b = 107.9960(10)°, V = 665.62(10) Å 3 , Z = 2. Compound 2 crystallizes in the triclinic, space group P1, with a = 5.2455(7) Å , b = 8.4637(11) Å , c = 12.0299(15) Å , a = 97.9620(10), b = 98.954(2)°, c = 95.1990(10), V = 519.04(12) Å 3 , Z = 1. Both supramolecular architectures of the compounds 1-2 involve O-HÁÁÁN/N-HÁÁÁO hydrogen bonds as well as CH-O interactions. The role of these noncovalent interactions in the crystal packing is ascertained. These weak interactions combined, both compounds displayed 3D framework structure.