Abstract: Developing highly efficient and stable photocatalyst for hydrogen evolution is of great significance, yet challenging. Herein, a strategy via chemically covalent combination between organic molecules is proposed for photocatalyst modification. And polyaniline-grafted CTF-1 composites (PANI-CTF-1) are prepared via such a chemically covalent combination strategy. Spectral characterizations indicate that PANI and CTF-1 are connected through —N—C=N— covalent bonds, which not only bridge the two components but also serve as a charge transfer channel between them, thus improving the transfer rate and injection efficiency of photogenerated charges. The photocatalytic experiments show that the as-prepared PANI-CTF-1 exhibits superior photocatalytic hydrogen evolution rate and higher stability as compared with the traditional PANI/CTF-1 heterojunction connected by van der Waals force.