New piperidine based ligands of the type [C5H10NCONR2] (where R=CH3 (L1), C2H5 (L2) and iC3H7 (L3)) have been prepared and characterized. The complex chemistry of these ligands with uranyl chloride, bromide, nitrate and β-diketonates has been studied using IR and NMR spectroscopic methods. Crystal structures for the complexes [UO2Cl2(L3)2] (1), [UO2Br2(L3)2] (2) [UO2(NO3)2(L3)2] (5) and [UO2(C4H3SCOCHCOCF3)2(L3)] (8) have been determined by the X-ray diffraction method. The structures of 1 and 2 show that the uranyl ion is surrounded by two of the ligands and two halogen atoms in an octahedral geometry. The structure of 5 shows that the uranyl group is surrounded by two nitrate groups and two ligands in a hexagonal bipyramidal geometry. The structure of 8 shows that the uranyl group is surrounded by two β-diketonates and one ligand in a pentagonal bipyramidal geometry. The structures show that the carboxamide ligands are strongly bonded to the uranyl group, showing a near linear geometry for the U–O–C bond (angle 150–159°). The prepared chloro and bromo compounds are air and moisture stable and show good solubility in normal organic solvents.