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The [Co(Me₂Salen)(PBu₃)(OH₂)]BF₄ and [Co(Me₂Salen)(PPh₃)(Solv)]BF_4, complexes were synthesized and characterized by FT-IR, UV–Vis, ¹H NMR spectroscopy and elemental analysis techniques. The coordination geometry of [Co(Me₂Salen)(PPh₃)(H₂O)]BF₄ was determined by X-ray crystallography. It has been found that the complex is containing [Co(Me₂Salen)(PPh₃)(H₂O)]BF₄ and [Co(Me₂Salen)(PPh₃)(EtOH)]BF₄ hexacoordinate species in the solid state. Cobalt atom exhibits a distorted octahedral geometry and the Me₂Salen ligand has the N2O2 coordinated environment in the equatorial plane. The [Co(Me₂Salen)(PPh₃)(H₂O)]BF₄ complex shows a dimeric structure via hydrogen bonding between the phenolate oxygen and hydrogens of coordinated H₂O molecule. These complexes were incorporated into Montmorillonite-K10 nanoclay. The modified clays were identified by FT-IR, XRD, EDX, TGA …