AbstractAtmospheric pollution has been recognized as a primary global emergency, especially in large cities and industrial areas. Among the most common harmful pollutants, nitrogen oxides (NOx) are responsible for a plethora of adverse effects, and their effective elimination from air has become an imperative task. In this regard, photocatalysis stands as an attractive technology for NOx degradation, provided that low‐cost and efficient visible ‐light photocatalysts are developed. In this regard, the construction of heterojunctions between energy band‐matched semiconductors is an effective strategy to boost the ultimate material photoactivity. In the present study, green heterocomposites based on MgAlTi layered double hydroxides (LDHs) and graphitic carbon nitride (gCN) are prepared using an amenable and cost‐effective route. A proper modulation of the system characteristics, as demonstrated by a comprehensive investigation, enabled to obtain very attractive DeNOx performances thanks to the efficient construction of MgAlTi/gCN heterojunctions with tailored features. The formation of the target heterocomposites significantly enhances the visible light photoactivity of the pristine LDH, boosting nitrogen monoxide transformation to nitrites/nitrates with a remarkable recycling stability. Overall, the presently reported results open the door to a profitable system exploitation for air purification under real‐world conditions, with considerable impact on both human wellbeing and environmental protection.