| Summary: | Two penta-coordinate Co<sup>II</sup> complexes with formulae [Co(14-TMC)Cl](BF<sub>4</sub>) (<b>1</b>, 14-TMC = 1,4,8,11-Tetramethyl-1,4,8,11-tetraazacyclotetradecane) and [Co(12-TBC)Cl](ClO<sub>4</sub>)·(MeCN) (<b>2</b>, 12-TBC = 1,4,7,10-Tetrabenzyl-1,4,7,10-tetraazacyclododecane) were synthesized and characterized. Structural analysis revealed that ligand coordinates to the Co<sup>II</sup> centre in a tetradentate fashion and the fifth position is occupied by chloride ion and the geometries around Co<sup>II</sup> centres are best described as distorted square pyramidal. Detailed magnetic measurements disclose the presence of significant easy-plane magnetic anisotropy and field induced slow magnetic relaxation behaviours of the studied complexes. More insight into the magnetic anisotropy has been given using <i>ab initio</i> theory calculations, which agree well with the experimental values and further confirmed the easy-plane magnetic anisotropy.
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