AbstractStabilization of zero-valent CuNi nanoparticles (NPs) supported on Cicer arietenum (CP) is reported here for the reduction and removal of persistent organic pollutants. The functional groups and interactions of NPs with the CP were determined by ATR-FTIR. The crystallinity, morphology, and the elemental composition of the samples were determined through powder XRD, FESEM, and EDS techniques, respectively. The XRD spectrum displayed a sharp crystalline peak at 43.9 for CuNi. The Cu and Ni zero-valent NPs displayed a peak at almost the same region, and thus, both the peaks are merged and appeared as a single peak. The chemical reduction/degradation of eight model pollutants, viz., 2-nitrophenol (ONP), 3-nitrophenol (MNP), 4-nitrophenol (PNP), 2,4-dinitrophenol (DNP), methyl orange (MO), congo red (CR), methylene blue (MB), and rhodamine B (RB) were carried out in the presence of NaBH4. The kapp value of 0.1 mM 4NP was highest which was 1.8 × 10−1 min−1 while the slowest rate was observed for CR and RB with kapp 5.5 × 10−3 and 5.4 × 10−3 min−1 respectively. This article helps in the removal of toxic organic pollutants through green supported NPs.