A magnetically separable cobalt complex of macrocyclic pseudo-crown ether (PCE) immobilized on magnetic Cu/Al-layered double hydroxide (γ-Fe 2 O 3 @Cu 3 Al-layered double hydroxide (LDH)/PCE-Co) was readily fabricated using a simple four-step postsynthetic modification strategy. This newly prepared nanocomposite was characterized by different chemo-physical approaches, including Fourier transform infrared (FT-IR), scanning electron microscopy (SEM), transmission electron microscopy (TEM), inductively coupled plasma optical emission spectroscopy (ICP-OES), vibrating sample magnetometer (VSM), X-ray diffraction (XRD), nitrogen adsorptiondesorption isotherms, energy-dispersive X-ray spectroscopy (EDX), and elemental mapping. The catalytic performance of these nanoparticles (NPs) was explored in the synthesis of diverse 1H-chromeno[2,3-b]pyridine-3-carbonitrile derivatives via one-pot three-component reactions under green reaction conditions. Environmentally benign reaction conditions, simple separation, high yields of the reactions, versatility, easy magnetic separation, and reusability for several runs without significant loss of catalytic performance are the key advantages that make this protocol an ideal alternative method for the synthesis of chromene derivatives.