We successfully prepared and characterized a distinctive thorium-based MOF (metal-organic framework) Th-TTHA with thorium oxide wheel clusters under the conditions of solvothermal synthesis by utilizing thorium nitrate and semirigid triazine hexacarboxylic acid linker H6TTHA (H6TTHA = 1,3,5-triazine-2,4,6-triamine hexaacetic acid). To the best of our knowledge, Th-TTHA is the first thorium-based MOF assembled by semirigid triazine hexapod ligand H6TTHA. It is worth mentioning that Th-TTHA exhibits a novel and distinctive arrangement of structure and topology. Th-TTHA has abundant adsorption sites such as the triazine ring that is rich in nitrogen atoms, N of NH-, and carboxyl oxygen atoms without coordination with a central metal, which drove us to explore its iodine adsorption capacity. The experimental results show that Th-TTHA shows excellent adsorption capacity for iodine, and the adsorption amount in a saturated iodine cyclohexane solution can reach 528 mg/g within 24 h. This work is greatly significant for the development of new structures of thorium-based MOFs and the expansion of its functional characteristics, which is very essential for our in-depth understanding of thorium chemistry and in the management and disposal of radionuclides and application of the nuclear fuel cycle.