Covalent　triazine　framework　(CTF)　is　widely　utilized　in　lots　of　porosity　related　applications　such　as　gas　storage,　molecule　separation　and　heterogenous　catalysis.　The　permanent　porosity　and　high　nitrogen　content　in　the　CTF　material　will　greatly　promote　the　affinity　between　gas　molecules　and　the　skeleton.　In　this　work,　four　covalent　triazine　framework　materials　(denoted　as　Py-CTF-400,　Py-CTF-500,　TPPy-CTF-400　and　TPPy-CTF-500)　with　high　BET　surface　areas　had　been　successfully　constructed　by　pyrene-based　building　block　under　ionothermal　reaction　conditions　using　anhydrous　ZnCl2　as　the　polycyclotrimerization　catalyst.　The　surface　area,　pore　volume/size　of　CTFs　can　be　simply　tuned　by　varying　the　synthesis　temperature.　Among　the　four　CTFs,　TPPy-CTF-400　display　high　specific　surface　area　up　to　1753　m(2)/g.　The　high　surface　area　and　nitrogen　rich　scaffold　enable　these　CTFs　to　facilitate　in　CO2/N-2,　CO2/CH4　separation.　Impressively,　the　CO2/N-2　selectivity　of　Py-CTF-500　is　up　to　45.3　(298　K,　1　bar),　which　is　comparable　to　the　highest　value　calculated　by　ideal　adsorption　solution　theory　(IAST)　among　CTF　based　materials.　More　importantly,　as　the　building　units　of　these　CTFs　extending　from　1,3,6,8-tetracyanopyrene　(TPy)　to　1,3,6,8-tetrakis(4-cyanophenyl)　pyrene　(TPPy),　their　CO2/N-2,　CO2/CH4　separation　efficiency　decreased,　which　is　probably　ascribed　to　the　decrescent　size　of　the　corresponding　pore　aperture.