Development　of　adsorbent　materials　for　highly　efficient　iodine　capture　is　high　demand　from　the　perspective　of　ecological　environment　and　human　health.　Herein,　the　two　kinds　of　thiophene-based　covalent　organic　frameworks　(COFs)　with　different　morphologies　were　synthesized　by　solvothermal　reaction　using　thieno[3,2-b]thiophene-2,5-dicarbaldehyde　(TT)　as　the　aldehyde　monomer　and　tri(4-aminophenyl)benzene　(PB)　or　tris(4-aminophenyl)amine　(PA)　as　the　amino　monomer　(denoted　as　PB-TT　COF　and　PA-TT　COF)　and　the　as-prepared　two　heteroatoms-rich　COFs　possessed　many　excellent　properties,　including　high　thermal　stability　and　abundant　binding　sites.　Among　them,　PB-TT　COF　exhibited　ultra-high　iodine　uptake　up　to　5.97　g/g　in　vapor,　surpassing　most　of　adsorbents　previously　reported,　which　was　ascribed　to　its　high　specific　surface　(1305.3　m(2)/g).　Interestingly,　PA-TT　COF　with　low　specific　surface　(48.6　m(2)/g)　showed　good　adsorption　ability　for　iodine　in　cyclohexane　solution　with　uptake　value　of　750　mg/g,　which　was　2.38　times　higher　than　that　obtained　with　PB-TT　COF　due　to　its　unique　sheet-like　morphology.　Besides,　the　two　COFs　possessed　good　reusability,　high　selectivity　and　iodine　retention　ability.　Based　on　experimental　results,　the　adsorption　mechanisms　of　both　COFs　were　studied,　revealing　that　iodine　was　captured　by　the　physical-chemical　adsorption.　Furthermore,　the　both　COFs　showed　excellent　adsorption　ability　in　real　radioactive　seawater　treated　safely,　demonstrating　their　great　potential　in　real　environment.　(c)　2022　Published　by　Elsevier　B.V.　on　behalf　of　Chinese　Chemical　Society　and　Institute　of　Materia　Medica,　Chinese　Academy　of　Medical　Sciences.