Abstract: The mixed-metal [(C4H9)4P][M(II)Cr(ox)3] M(II) = Mn(1), Fe(2), Co(3), Ni(4), Cu(5) and ox is oxalate, has been prepared. X-ray powder diffraction patterns and their Rietveld refinement show that all the compounds along the series are isostructural and single-phased. X-ray powder diffraction profiles are indexed in hexagonal and P63 space group. The magnetic susceptibility data obey Curie-Weiss law in temperature 300-5 K with a positive constants of 15.1 (1), 13.5 (2), 12.7 (3), 12.0 (4) and 11.0 K (5). The temperature dependence of the molar magnetization exhibits a magnetic phase transition at Tc = 12 K (1), 11 (2), 10 (3), 8(4), 7 K (5). At low temperature, the compounds complex exhibit long-range ordered magnetic behavior.