Four new Cu(II) Complexes viz. [Cu(II)(1-amidino-O-methylurea) 2 ]SO 4 ·2H 2 O (1), [Cu(II)(1-amidino-O-ethylurea) 2 ](SO 4 ) 2 ·2H 2 O (2), [Cu(II)(1-amidino-O-n-propylurea) 2 ] SO 4 ·2H 2 O (3), [Cu(II)(1-amidino-O-n-butylurea) 2 ] 2 (SO 4 ) 2 ·2H 2 O (4) have been synthesized and characterized. EPR spectrum of complex 4 at RT consisted of fine-structure transitions (ΔMs=±1) with zero-field splitting (ZFS) of 0.0485cm −1 and a half-field signal (ΔMs=±2) at ca. 1600G, revealed formation of binuclear complex (S=1). Whereas EPR spectrum of complex 2 in DMSO showed a mixture of mononuclear and binuclear complex in the ratio 0.75:1.0 with ZFS of 0.0385cm −1 . From the temperature dependence of the EPR signal intensity, the isotropic exchange-interaction constant J was evaluated.