Composition space has been used to study the phase stability of organically templated uranium sulfates in the UO2(CH3CO2)(2).2H(2)O-1,3-diaminopropane-H2SO4 system. The syntheses and structures of two new compounds, [N2C3H12][UO2(H2O)(SO4)(2)] (USO-1) and [N2C3H12][(UO2)(2)(H2O)(SO4)(3)] (USO-2), are reported. The relative stability of the crystalline products in this system was found to be dependent upon the reactant mole fraction in the initial reaction gel, based upon the size and location of their respective crystallisation fields in the composition space.