Abstract
ABSTRACT
Expanded light absorption and optimized heterostructure interfaces can significantly enhance photocatalytic redox performance. Herein, perovskite CsPbI
3
nanocrystals (NCs) and nanowires (NWs) are integrated with graphitic carbon nitride (g‐C
3
N
4
) nanosheets via a combined mechano‐chemical pre‐reaction and solvothermal process. This strategy effectively removes surface ligands and enables the formation of well‐defined heterostructures with strong interfacial contact, facilitating efficient charge carrier transfer. The distinct morphologies and band structures of CsPbI
3
NCs and NWs lead to differentiated photocatalytic behaviors in CO
2
reduction and NO removal. An S‐scheme charge transfer mechanism further promotes charge separation and migration. Among the composites, g‐C
3
N
4
/CsPbI
3
NWs exhibit superior CO
2
reduction activity, achieving a visible‐light‐driven CO production rate of 4.6 µmol g
−1
h
−1
, attributed to the face‐to‐face interface and one‐dimensional architecture that enhance charge transport. In contrast, g‐C
3
N
4
/CsPbI
3
NCs demonstrate excellent NO removal performance, with a removal efficiency of 69.5% and low NO
2
selectivity (5.0%) at 600 ppb NO, owing to the generation of high‐energy photoinduced charge carriers. This work presents a versatile design strategy for g‐C
3
N
4
‐based photocatalysts toward efficient energy conversion and environmental remediation.