Nitroanilines are environmentally toxic pollutants which are released into aquatic systems due to uncontrolled industrialization. Therefore, it is crucial to convert these hazardous nitroanilines into a harmless or beneficial counterpart. In this context, we present the chemical reduction of 4-nitroaniline (4-NA) by NaBH 4 utilizing Prussian blue analogue (PBA) as nanocatalyst. PBAs can serve as inexpensive, eco-friendly, and easily fabricated nanocatalysts. PBA cobalt tetracyanonickelate hexacyanochromate (CoTCNi/HCCr) was stoichiometrically prepared by a facile chemical coprecipitation. Chemical, phase, composition, and molecular interactions were investigated by XRD, EDX, XPS, and Raman spectroscopy. Additionally, SEM and TEM micrographs were utilized to visualize the microstructure of the nanomaterial. The findings revealed the synthesized PBA of the cubic phase and their particles in nanosheets. The band gap was estimated from the optical absorption within the UV−vis region to be 3.70 and 4.05 eV. The catalytic performance of PBA for the reduction of 4-NA was monitored by UV−vis spectroscopy. The total reduction time of 4-NA by PBA was achieved within 270 s, and the computed rate constant (k) was 0.0103 s −1 . The synthesized PBA nanoparticles have the potential to be used as efficient nanocatalysts for the reduction of different hazardous nitroaromatics.