Two organic salts (4-phenylthiazol-2-amine)(2):(sulfuric acid) [(HL1(+))(2)center dot(SO4 (2-))]center dot C2H5OH center dot H2O (1), and (4-phenylthiazol-2-amine):(hydrochloride acid) [HL1(+)center dot(Cl-)]center dot H2O (2) based on 4-phenylthiazol-2-amine (L1) were prepared and structurally characterized by X-ray crystallography. Compound 1 crystallizes in the monoclinic, space group C2/c, with a = 22.329(2) , b = 9.6580(10) , c = 24.484(3) , beta = 113.528(2)A(0), V = 4841.1(9) (3), Z = 8. For 1, the cations were connected through H2O molecules and the sulfate anions to form a 1D chain running along the b axis direction. Two such adjacent chains were joined together through pi-pi and O-H center dot center dot center dot O interactions along the c axis direction to generate a double chain structure. The double chains were further connected by N-H center dot center dot center dot O, N-H center dot center dot center dot S, and O-S interactions to form tetra-chain structure. The cations also form dimers via pi-pi interactions. On every chain of the tetramers there were bonded the cation dimers through C-H center dot center dot center dot O interactions. The cation dimers were sandwiched between the tetra-chains to form a 3D ABAB layer structure when viewed along the a axis direction. Compound 2 crystallizes in the monoclinic, space group P2(1)/c, with a = 12.6604(12) , b = 9.1400(8) , c = 10.1263(11) , beta = 110.2230(10)A(0), V = 1099.54(19) (3), Z = 4. In 2, the cations were connected by N-H center dot center dot center dot Cl, and S-Cl interactions to form a 1D chain extending along the b axis direction. Two neighboring chains were further connected by N-H center dot center dot center dot Cl hydrogen bonds to form a double chain structure. Adjacent double chains were stacked along the a axis direction through O-H center dot center dot center dot Cl hydrogen bonds to form a 3D layer network structure.