U60 (Li44K16[UO2(O2)(OH)]60, U60) and polymers are directionally enriched on the polymer surface by hydrogen bonding. In this study, we used several different polymers and U60 for self-assembly. The morphology and non-covalent interaction between core-shell nanocomplexes were studied by electron microscopy and vibration spectroscopy. Under the synergistic action of hydrogen bonding and nanometer phase separation, block copolymers and U60 formed different structures of core-shell nanocomposites. At a low concentration of U60, spherical nanocomposites with frozen structures were formed, at a high concentration of U60, stable worm-like structures, and micelles were formed. We used block copolymers to absorb U60, and after one month, about 96% of U60 could be removed from the solution. Because of uranium toxicity and long half-life, storage and transportation are important for the environment and public health. This study may open the door for further development of novel and efficient polymer self-assembly materials to adsorb and remove nuclear pollution in the environment.