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High-yield selective adsorbents and suitable modification methods are both significant for the efficient treatment of U-contaminated wastewater. In this work, a rich-mesoporous aluminum phosphate adsorbent (APO-10) was synthesized by simply increasing the mass of reactants under a fixed solvent volume. After increasing the mass of reactants ten times, APO-10 has the added defect level, the increased specific surface area, and mesoporous structure, and the increased number and enhanced adsorption ability of adsorption active sites (phosphorus-oxygen groups) on the surface, resulting in an enhanced adsorption performance of U(VI) in various environmental conditions. Its ultrahigh adsorption capacity calculated by the Langmuir model can reach 826.44 mg g−1 at pH = 5.5 and T = 298 K. Its crystal structure did not change after adsorption and remained at 584.40 mg g−1 after 6 cycles. Additionally, APO-10 shows an excellent uranium-selectivity over 68% from a mixed aqueous solution and has excellent applicability in the acidic and alkaline environment based on dynamic adsorption and desorption column experiments. This study not only provides a high-yield efficient selective adsorbent (APO-10) with excellent anti-radiation structure stability for the treatment of radioactive contamination but also provides a feasible modification method by simply increasing the mass of reactants. [Display omitted] • A high-yield adsorbent (APO-10) was synthesized by increasing the raw materials. • The physicochemical properties of the adsorbent changed after added raw materials. • The increased adsorption capacity of APO-10 for U(VI) reaches 826.44 mg g−1. • APO-10 shows the enhanced uranium-selectivity from a mixed aqueous solution. • APO-10 has excellent structural stability and enhanced recycling performance. [ABSTRACT FROM AUTHOR]