The first four uranyl peroxide compounds containing ethylenediaminetetra-acetate (EDTA) were synthesized and characterized from aqueous uranyl peroxide nitrate solutions with a pH range of 5-7. Raman spectra demonstrated that reaction solutions that crystallized [NaK15[(UO2)(8)(O-2)(8)(C10H12O10N2)(2)(C2O4)(4)].(H2O)(14)] (1) and [Li4K6[(UO2)(8)(O-2)(6)(C10H12O10N2)(2)(NO3)(6)].(H2O)(26)] (2) contained excess peroxide, and their structures contained oxidized ethylenediaminetetraacetate, EDTAO(2)(4)-. The solutions from which [K-4[(UO2)(4)(O-2)(2)(C10H13O8N2)(2)(IO3)(2)].(H2O)(16)] (3) and LiK3[(UO2)(4)(O-2)(2)(C10H12O8N2)(2)(H2O2)(2)].(H2O)(18) (4) crystallized contained no free peroxide, and the structures incorporated intact EDTA(4)-. In contrast to the large family of uranyl peroxide cage clusters, coordination of uranyl peroxide units in 1-4 by EDTA(4)- or EDTAO(2)(4)- results in isolated tetramers or dimers of uranyl ions that are bridged by bidentate peroxide groups. Two tetramers are bridged by EDTAO(2)(4)- to form octamers in 1 and 2, and dimers of uranyl polyhedra are linked through iodate groups in 3 and EDTA(4)- in 4, forming chains in both cases. In each structure the U-O-2-U dihedral angle is strongly bent, at similar to 140 degrees, consistent with the configuration of this linkage in cage clusters and other recently reported uranyl peroxides.