Designing Efficient MoS 2 /g‐C 3 N 4 Hybrid Photocatalysts by Regulating the Interlayer Spacing of MoS 2

g‐C 3 N 4 as an appealing photocatalyst has received much attention due to its abundance, nontoxicity, and unique photoelectric properties. However, bare g‐C 3 N 4 usually suffers from restricted light absorbance and serious carriers recombination. The key issue of boosting the photocatalytic performance of the g‐C 3 N 4 lies in constructing hybrids for better optical and electrical effects. Here, the MoS 2 with different interlayer spacing is integrated with g‐C 3 N 4 via calcination and hydrothermal methods to form the high‐performance MoS 2 /g‐C 3 N 4 hybrid photocatalyst. Optimized energy‐band alignment with g‐C 3 N 4 is realized through regulating the interlayer spacing of MoS 2 , achieving improved carriers separation efficiency. In addition, the broadband absorption and rich active sites are also achieved here. As a result, the rationally designed MoS 2 /g‐C 3 N 4 composite (the MoS 2 interlayer spacing: 1.02 nm) exhibits the dominant photocatalytic performance (hydrogen production rate: 1281 μmol/h/g). This work opens a new road to realize a proper energy‐band alignment with g‐C 3 N 4 for high performance photocatalytic activity.