Presented here are two isostructural uranyl coordination polymers [UO_2(EDO)(H_2O)]?H_2O(1) and [UO_2(BDO)(H_2O)]?2H2_O(2)(EDO~(2-)=ethylene-1,2-dioxamate; BDO~(2-)=butylene-1,2-dioxamate) with identical stepwise zigzag chain structure and distinct interchain hydrogen bonding interaction, prepared from hydrothermal reaction of DEEDO or DEBDO(DEEDO= diethyl ethylene-1,2-dioxamate; DEBDO=diethyl butylene-1,2-dioxamate) with uranyl ions. The monomeric uranyl-based fluorescence emissions of compounds 1 and 2 are red-shifted by about 6 and 5 nm respectively, compared to that of uranyl nitrate hexahydrate. Compound 1 has stronger emission than compound 2, but both their emissions exhibit triple-exponential decay. The photophysics of uranyl oxalate trihydrate was also investigated for comparison. The selective crystallization of compound 1 in alkaline solution was applied to the sequestration of uranyl ions, showing a kinetic preference. Presented here are two isostructural uranyl coordination polymers [UO_2 (EDO) (H_2O)] H_2O (1) and [UO_2 (BDO) (H_2O)] 2H_2_O (2) (EDO ~ -dioxamate; BDO ​​~ (2 -) = butylene-1,2-dioxamate) with identical stepwise zigzag chain structure and distinct interchain hydrogen bonding interaction, prepared from hydrothermal reaction of DEEDO or DEBDO (DEEDO = diethyl ethylene- ; DEBDO = diethyl butylene-1,2-dioxamate) with uranyl ions. The monomeric uranyl-based fluorescence emissions of compounds 1 and 2 are red-shifted by about 6 and 5 nm respectively, compared to that of uranyl nitrate hexahydrate. Compound 1 has stronger emission than compound 2, but both their emissions exhibit triple-exponential decay. The photophysics of uranyl oxalate trihydrate was also investigated for comparison. The selective crystallization of compound 1 in alkaline solution was applied to the sequestration of uranyl ions, showing a kinetic preference.