Three (3,4)-connected uranyl-organic frameworks (UOFs) with pto and tbo topologies were synthesized. The UOF with a pto net possesses a 2-fold interpenetrating network and exhibits 2D interconnected channels. The UOF with a tbo net is constructed from two types of ultralarge nanocages. All these compounds can efficiently remove large cationic dye crystal violet (CV) through a cation exchange mechanism.