Neodymium-doped Zn–Al layered double hydroxide (Nd/Zn-Al LDH) with excellent photocatalytic activity was prepared by a one-step hydrothermal method. The morphology and physicochemical properties of as-synthesized photocatalysts were well analyzed by Fourier transform infrared (FT-IR), X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), photoluminescence (PL), UV-diffuse reflectance spectroscopy (UV-DRS), and Brunauer-Emmett-Teller (BET) surface analysis. Doping Nd3+ into Zn–Al LDH enhances the overall catalytic activity of the nanocomposite, like better electron–hole pair separation, increase in interplanar distance, fast electron transfer, and large surface area. The as-prepared nanocomposite shows excellent degradation of three different dyes under visible light irradiation. The degradation efficiency of these dyes follows the order of Congo red > rose Bengal > fast green. Furthermore, liquid chromatography-mass spectrometry (LC-MS) was employed to propose a possible photocatalytic degradation pathway for Congo Red and Rose Bengal dyes by Nd/Zn–Al LDH. With the help of radical trapping experiments, it is revealed that during the photoexcitation process, the primary reactive intermediates are hydroxyl radicals. Display omitted