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The syntheses, structural characterization, and magnetic behavior of two new hexanuclear copper(II) complexes derived from R-phosphonic acids and 1,3-bis(dimethylamino)-2-propanol (Hbdmap) with formulas [Cu6,(µ-bdmap)3(µ3Ph-PO3)2(µ3-O···H···µ3-O)(ClO4)2(H2O)]5H2O (1) and [Cu6(µ-bdmap)3(µ3-t-Bu-PO3)2(µ3-O···H···µ3-O)(µ1,3-dca)(dca)-(H2O)]6H2O (2) (Ph-H2PO3 = phenylphosphonic add, t-Bu-H2PO3 = tert-butylphosphonic acid, dca(dicyanamide) are reported. Compounds 1 and 2 are hexanuclear 3.111 R-phosphonate(2-)/1,3-bis(dimethylamino)-2-propanolato(1-) cages including in the center the [µ3–O···H···µ3–O]3- unit. The temperature dependence of the magnetic properties of 1 and 2 dearly indicates an overall strong antiferromagnetic coupling confirmed by DFT calculations. [ABSTRACT FROM AUTHOR]