Porous organic frameworks may be a kind of promising material to address environmental issues such as removing the radioactive vapor wastes in fission as well as coping with organic pollutants of wastewater, due to their excellent porous character and remarkable stability. In this report, a covalent triazine-based framework (CTF-CTTD) with hierarchically porous structure and large pore volume was synthesized via the nitrile trimerization. The CTF-CTTD shows an outstanding adsorption ability for iodine with the uptake value of 387% due to their abundant porosity, triazine units, as well as pi-pi conjugated structures, which is one of the highest values reported so far for iodine uptake values of solid porous adsorbents. Furthermore, iodine captured in CTF-CTTD can be also released easily from the pore of materials because of the highly porous structure. In addition, CTF-CTTD also presents an excellent adsorptive performance for removing Rhodamine B (RhB) with adsorption capacity of 684.9 mg g(-1).These results obtained may provide a guidance for the design of adsorbent with high specific surface area and large pore volume as well as the hierarchically porous structure in capturing of radioactive iodine and removing RhB from wastewater.