Uranium enrichment and separation are important for the sustainable development of nuclear energy. In this study, reverse-phase emulsion crosslinking polymerization was used to synthesize spherical hollow porous carbon materials (II-CLSPC) with a “red blood cell” morphology after roasting. The soft template method was used to modify II-CLSPC to obtain an open pore structure, which increased its contact area. Based on this, ion imprinting was conducted to improve the selective adsorption of U(VI). A spatial site matching the size of U(VI) was formed after ion template removal, which played a crucial role in this process. Multifaceted and multilevel improvements of II-CLSPC facilitated rapid adsorption, reaching equilibrium at 40 min and a removal rate of 94.6 % (pH 5, 298 K). The pseudo-second-order kinetic model and Langmuir isothermal model indicated that the adsorption process of uranyl ions by II-CLSPC involved via monolayer chemisorption with a theoretical saturation adsorption capacity of 653.6 mg g−1. In addition, II-CLSPC exhibited excellent selectivity (KdU = 3.7 × 104 mL g−1), cyclic stability, and salt tolerance, making it a promising candidate for uranium removal from wastewater.