In this paper, a novel nanocomposite was prepared as a heterogeneous catalyst using layered double hydroxide (LDH), and copper(II) nanoparticles stabilized on guanidine (Mg-Al LDH@Guanidine-Cu(II)) (1). This nanocomposite was used in multi-component reactions for the synthesis of 2-(1H-tetrazole-5-yl) acrylonitrile derivatives with high yield in short reaction times. Identification of this nanocatalyst was performed by FT-IR, EDS, FE-SEM, TEM, XRD and TGA techniques. This nanocatalyst showed high thermal stability, high specific surface area, and good reusability up to 4 times without significant loss of activity. In addition, excellent activity, easy separation, and milder reaction conditions are among the factors that make this nanocomposite an excellent catalytic system for these reactions. In addition, synthesis of 2-(1H-tetrazole-5-yl) acrylonitrile derivatives under green chemistry conditions was performed using various benzaldehyde derivatives, malononitrile, sodium azide, and the optimal amount of nanocatalyst. The support used in this nanocatalyst was LDH which have become popular in the field of heterogeneous catalysts due to its very easy and low cost synthesis as well as excellent combination of structural features such as abundant hydroxyl groups on the surface, tunability of host layers, interlayer anions, regular distribution of metal cations, etc.