In this work the ability of ZnAlFe-CO₃ layered double hydroxides (LDHs) as highly efficient UV–Vis light photocatalysts for the photochemical oxidation of NO gas was studied. LDHs with 3.5 to 4.1 M²⁺/M³⁺ and 0.33 to 1.55 Fe/Al ratios were prepared by a coprecipitation method. The samples were characterized by different techniques such as XRD, XPS, FT-IR, ICP-MS, TG, SBET, SEM and Diffuse reflectance (DR). The increased presence of the Fe³⁺ ions gave rise to changes in the structure, morphology and optical properties of the LDHs. The prepared ZnAlFe-CO₃ systems exhibited increased surface area and enhanced visible-light absorbance. The photochemical NO abatement resulted in outstanding conversion efficiency (56%) and selectivity (93%) for the iron containing samples, due to a decrease of the e^-/h⁺ recombination, higher generation of radical dotO₂^– and radical dotOH radicals and their NO₂ adsorption ability.