In this report, a new precursor binuclear complex of Zn(II) and Ni(II) ions under formula [Zn(phen)(L)(OH2)(µ-SCN)Ni(phen)(L)(SCN)](1) that phen=1-10-phenanthroline, L=2-aminobenzoate has been synthesized and then the facile synthesis of Ni-Zn-NPs has been reported under thermal decomposition. The complex (1) was characterized using cyclic voltammetry (CV), elemental analysis, and spectroscopic methods (IR, UV-Vis). FT-IR spectrum of complex (1) show vibrational frequency of NH group of anthranilic acid ligand appeared in the 3421 cm-1. UV–visible spectrum of the compound (1) show d-d transitions of Ni(II) ion. Characterization of the nano-particle was performed with scanning electron microscopy (SEM), FT-IR spectroscopy, and X-ray powder diffraction (XRD). The X-ray diffraction pattern showed a pure system Ni0.9Zn0.1O with a monoclinic structure. The average particle size was 27 nm using the Debye- Scherrer equation. Finally, the nano-particle has been used as a catalyst for the preparation of tetrahydrobenzo[b]pyran. The best datas were achieved when the reaction was carried out at 60 °C in the presence of Ni0.9Zn0.1O (5 mol %) in 2:1 EtOH/H2O.