There is a strong need for the development of effective uranium sorbents. Here, the Friedel-Crafts reaction was performed in a simple one-step manner followed by phosphate esterification to prepare porous hyper-cross-linked Bisphenol F (PHCP-BF) for prospective utilization in the removal of U(VI) from wastewater. PHCP-BF has pores with a size of 2.6 nm and a significant BET surface area (up to 387.31 m2/g). It was extensively investigated how a variety of environmental conditions (e.g., pH, contact time, temperature, etc.) affected the treatment results. In terms of adsorption capacity, uranium possessed a maximum of 120 mg/g (pH = 7), which is twice that of the original material HCP-BF (59.39 mg/g). According to the modeling results, with the Langmuir isotherm and a pseudo-second-order kinetic model, the data matched the sorption data very well. It was found that PHCP-BF possessed good selectivity for uranium, which was considerably greater than that of other co-existing metals. After three cycles, PHCP-BF still maintained a certain adsorption capacity. In light of several spectroscopic examinations, the mechanism of uranium removal by PHCP-BF is the chelated of P = O with U (VI). The results obtained suggest that PHCP-BF can be used effectively to remove uranium from water.