A set of unique triptycene-based and organic Schiffbase-linked polymers (TBOSBLs) are conveniently synthesized in which triptycene motifs are connected with 1,3,5-triformylphloroglucinol units via Schiff-base linkages. TBOSBLs are amorphous, thermally stable with a reasonable surface area (SA BET up to 649 m 2 /g), and have abundant nanopores (pore size < 100 nm). TBOSBLs are good sorbents for small gas molecules (such as CO 2 , H 2 , and N 2 ) and they can selectively capture CO 2 over N 2 . Additionally, TBOSBLs show superior antiproliferative activity against human colorectal cancer cells relative to previously reported covalent organic frameworks (COFs). The mechanism of cell death is also studied elaborately.