Eutrophication of water bodies caused by the excessive phosphate discharge has constituted a serious threat on a global scale. It is imperative to exploit new advanced materials featuring abundant binding sites and high affinity to achieve highly efficient and specific capture of phosphate from polluted waters. Herein, water stable Zr-based metal organic frameworks (MOFs, UiO-66) with rational structural design and size modulation have been successfully synthesized based on a simple solvothermal method for effective phosphate remediation. Impressively, the size of the resulting UiO-66 particles can be effectively adjusted by simply altering reaction time and the amount of acetic acid with the purpose of understanding the crucial effect of structural design on the phosphate capture performance. Representatively, UiO-66 particles with small size demonstrates 415 mg/g of phosphate uptake capacity, outperforming most of the previously reported phosphate adsorbents. Meanwhile, the developed absorbents can rapidly reduce highly concentrated phosphate to below the permitted level in drinking water within a few minutes. More significantly, the current absorbents display remarkable phosphate sorption selectivity against the common interfering ions, which can be attributed to strong affinity between Zr–OH groups in UiO-66 and phosphate species. Furthermore, the spent UiO-66 particles can be readily regenerated and reused for multiple sorption–desorption cycles without obvious decrease in removal performance, rendering them promising sustainable materials. Hence, the developed UiO-66 adsorbents hold significant prospects for phosphate sequestration to mitigate the increasingly eutrophic problems.