The new complex of 2, 4, 6-trimethylpyridine (TMPy) cobalt chloride consists of CoCl4 anionsand trimethylpyridine cations by ionic electrostatic force. This complex belongs in space group of P21/c,having crystalline parameters of a = 8.915, b = 17.339, c = 13.945 Å, b = 102.54°, Z = 4 and Dm = 1.37Mg·m. Electronic structure calculation results indicated stronger covalence of (CoCl4)2- and demonstratedthat the coordination compound of CoCl4·(HTMPy)2 is very stable. There are positive charges on

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... 2, C4and C6 positions, and negative charges on C3 and C5 positions in pyridine ring. Mulliken bond grade andatom net charge were derived.