In order to search effective adsorbents for removal of metal ions in water treatments, three nanoporous organic frameworks, TPPA, TPPA-SO 3 H, and TPBD-SO 3 H, with or without −SO 3 H functionalities were selected and synthesized by the Schiff base reactions of 1,3,5-triformylphloroglucinol (TP) and p-phenylenediamine (PA), p-phenylenediaminesulfonic acid (PA-SO 3 H), and 2,2′-benzidinedisulfonic acid (BD-SO 3 H), respectively. Characterizations revealed that both TPPA and TPPA-SO 3 H possess high crystallinity and porosity, while only amorphous powder with irregular pores of TPBD-SO 3 H was obtained. The Brunauer−Emmett−Teller surface areas of 425.3 and 297.5 m 2 /g for TPPA and TPPA-SO 3 H, respectively, were calculated, while only 45.1 m 2 /g was detected for TPBD-SO 3 H. Metal ion adsorption experiments revealed that among all three framework materials, TPPA-SO 3 H shows the best performances in adsorption capacities, removal efficiency, and adsorption rate to all of the tested metal ions, especially Fe 3+ , Cr 3+ , and Cd 2+ ions. Compared with the absence of −SO 3 H functionalities in TPPA and the amorphous nature of the extended framework material of TPBD-SO 3 H, the high performances of TPPA-SO 3 H should be ascribed to its synergistic effect of functionalization and crystallinity. This study revealed that besides the functional groups, the crystallinity of nanoporous organic frameworks is also a crucial factor in their applications.