In order to protect environment and save uranium resources, it was necessary to find a highly efficient adsorbent for uranium recovery from wastewater. In this work, we used a freeze-drying-calcination method to synthesize HAP aerogel to effectively remove uranium. Compared with commercially available nano-hydroxyapatite, HAP aerogel presented better adsorption performance. This was because the as-prepared HAP aerogel presented continuous porous structure, which could provide more active sites for the adsorption to uranium. The uranium removal efficiency of HAP aerogel arrived 99.4% within 10 min and the maximum adsorption capacity was up to 2087.6 mg g−1 at pH = 4.0 and 298 K. In addition, the immobilization of uranium on HAP aerogel was chemisorption, which was probably due to adsorption, dissolution-precipitation and ions exchange. These results indicated that the as-prepared HAP aerogel could be widely used as a high efficiency and potential adsorbent for the treatment of uranium-containing wastewater in the future.