Two new uranyl sulfates, (C4H14N2)(UO2)2(SO4)3(H2O)·2H2O (NDUS2) and (C4H14N2)(UO2)(SO4)2(H2O)·2H2O (NDUS3), were synthesized and their crystal structures determined. NDUS2 was obtained in highly acidic media heat-treated at 373K and subsequently maintained at 278K until crystals formed after two months. NDUS3 results from the degradation of NDUS2 over the course of a few days. NDUS2 and NDUS3 crystallize in the monoclinic space group P21/n, a=10.9075(4)Å, b=10.4513(4)Å, c=17.7881(7)Å, β=97.908(2)°, V=2008.52(13)Å3, Z=4, at 140K and a=8.8570(4)Å, b=7.3299(3)Å, c=20.4260(9)Å, β=95.140(2)°, V=1320.74(10)Å3, Z=4, at 140K, respectively. The compounds contain interlayer 1,4-n-butyldiammonium cations that charge-balance the anionic structural units. Amine templating effect absent in uranyl sulfates synthesized with 1,4-diaminobutane, as shown by the synthesis of two new uranyl sulfates, (C4H14N2)(UO2)2(SO4)3(H2O)·2H2O (NDUS2) and (C4H14N2)(UO2)(SO4)2(H2O)·2H2O (NDUS3) Display omitted . ► Two layered uranyl sulfates were synthesized. ► Amine molecules are located in the interlayers of the compounds. ► No templating effect of the amine was observed. ► Amine molecules are only charge balancing cations in the structures.