Developing visible light responsive photocatalysts with strong light capture ability for catalytic NO removal is of great significance. In this work, we coupled the narrow-gap semiconductor BiOI with graphite-like carbon nitride (g-C3N4) to construct 2D/3D heterostructure and applied it for efficient photocatalytic elimination of NO under visible light irradiation. At relative humidity (RH) of 15 %, g-C3N4/BiOI achieves remarkable NO removal activity (80.5 %) under a gas hourly space velocity (GHSV) of 1,740,000 mL h−1 g−1. Outstanding durability was realized that the NO removal efficiency of g-C3N4/BiOI after 6 consecutive runs. Even at high RH of 50 % and 80 %, g-C3N4/BiOI still exhibited excellent NO removal performances of 80.3 % and 78.5 %, respectively. The heterostructure of g-C3N4/BiOI endowed the enhanced light harvesting, efficient charge separation and rapid charge transfer, which enables sufficient superoxide radicals (O2−) production to improve the efficiency and strengthen the durability of photocatalytic NO removal. This work provides insights into the rational design of heterostructure photocatalyst toward air purification.