In recent years, the synthesis and application of green, cost-effective, and sustainable materials for uranium (VI) removal was significant to environmental protection. The ordered mesoporous carbon (CMK-3) supported different mass of hydroxyapatite materials (HAP@CMK-3) were facilely synthesized via hydrothermal method. The resultant materials were characterized by XRD, FT-IR, BET, SEM, TEM mapping, and XPS, and implemented for immobilizing U(VI). Not only the specific surface area of HAP (7.01 m2/g) was increased by the loading on CMK-3 (818.37 m2/g), but also the adsorption capacity of CMK-3 was increased by HAP modification. Impressively, HAP@CMK-3 exhibited highly adsorption capacity of U(VI) with the increase of HAP deposition and was capable of achieving fast reaction. Therein to, the specific surface area of HAP@CMK-3(2:1) was 253.68 m2/g, as well as the adsorption capacity was up to 1072 mg/g (fitted by Langmuir isotherm, at pH=3.0, 298 K) and the adsorption process was completed in 30 min (followed by pseudo-second-order kinetic). The adsorption mechanisms of U(VI) on HAP@CMK-3 involved electrostatic forces, ionic interactions, and chemical complexation. This work offered new avenues to address the limitations of cost and less secondary pollution for the removal of U(IV) from wastewater.