Uranium (as a hazardous and radioactive element) removal from wastewater requires reliable technology and proper functional materials. Carbon fiber species that are produced from agricultural solid waste can be a proper type of low-cost adsorbents for wide uses in wastewater treatment. In this work, two carbon fiber species labeled CF-RH and CF-SCB were synthesized from two different agricultural wastes, namely, rice husk and sugarcane bagasse respectively. The structural properties of carbon fiber were verified by XRD, FTIR, and Raman, spectroscopy. Both nitrogen-adsorption–desorption BET surface area and TEM were performed to figure out the textural characteristics of the presented sorbents. The charges on surfaces of the fibers were detected via zeta potential analysis. The prepared carbon fibers were applied for uranium removal from aqueous solution by adsorption technique. The acquired data display that the equilibrium time was 240 min. The results of adsorption process are nicely fitted with pseudo-second-order-kinetic and Langmuir isotherm models. The maximum sorption capacity was 21.0 and 29.0 mg/g for CF-RH and CF-SCB, respectively. Sorption thermodynamics declare that adsorption of U(VI) is an endothermic, spontaneous, and feasible process. The picked findings of this study could emphasize high reliability of the introduced adsorbents in efficient tackling of water contaminants.