Methyl group tuning crystalline covalent triazine frameworks towards organogel

Covalent triazine frameworks (CTFs), known as highly conjugated layered solids, have garnered significant interest due to their distinctive structural and property characteristics. However, the exfoliation of CTF solids towards nanoCTFs in high yields is currently inadequate and inefficient, limiting their utility. This study presents the design and synthesis of CTFs containing non‐crystalline regions and their random stacks using a methyl‐containing nitrile monomer. Incorporating in‐plane methyl groups enhances the polarity of CTFs and disrupts layered interactions, facilitating smooth exfoliation under competing solvent‐layer interactions and producing nanocolloids in dilute dispersions. Furthermore, CTFs can rapidly disperse in DMF at a high concentration, enabling the formation of CTF organogel for the first time. Additionally, the designed CTF nanocolloids allow for the first simple physical modification of carbon nanotubes. The assembly, associated with conjugated features, enables the fabrication of CTF/carbon nanotube organogel.