Two novel crystal structures containing tetrahydrofuran-2,3,4,5-tetracarboxylic acid (THFTCA) and the uranyl (VI) cation were synthesized and characterized with single crystal X-ray diffraction and Raman spectroscopy. THFTCA is important in separating uranium from other actinides and is used in the disposal process of radioactive waste. This study analyzed how the coordination environment of the uranyl cation impacted its interactions with THFTCA. Two uranyl structures were isolated. The first, a simple monomer with piperazine acting as a charge balancing counter-cation. The second a framework with two unique uranyl environments and a sodium dimer. Within the uranyl structures, an increase in complexity was observed when a non-organic counter-cation was introduced, which contributed to the formation of a 3D framework. Shifts in the Raman spectra were analyzed to determine vibrational differences that resulted from the coordination of THFTCA to the uranyl cation.