CMPs and COFs, the CTFs reported in this work, are among the materials with the highest activity in HER under comparable conditions, e.g. basic conditions and TEOA as sacrificial electron donor (see Table ). Comparing to the only bipyridine-containing CTF reported up to date, CTF-HUST-C6, a crystalline material synthesized from condensation between terephthalamidine chloride and 5,5'-di(hydroxymethyl)-2,2'-bipyridine, similar catalytic activities are obtained (~6.5 mmol/g cat /h, Table , entry 10). In comparison to CTF-02 materials prepared by the TfOH-mediated polycondensation approach, we observe here an HER rate of up to one order in magnitude higher, under very similar catalytic conditions (4.3 mmol/g cat /h vs. ~0.3 mmol/g cat /h, 5 ). The material possess similar surface areas around 570 m 2 /g and bandgaps (~ 2.8 eV). We note however, that a direct comparison between different materials, even with very similar structure as in the case of the CTF-02 materials, is complex, as not only the band-gap and surface area affect the catalytic activity. As demonstrated above, in particular the precise positioning of the absolute frontier orbitals, the dynamics of photo response and the solvent-solid interactions (wettability, hydrophilicity) have a marked influence on a material's performance, and yet these parameters are scarcely reported CONCLUSION.