Selective aerobic oxidation of benzylamine to N,Nbenzylidenebenzylamine was achieved using a bismuth ellagate (Biellagate) metal-organic framework (MOF) under simulated visible light irradiation. The bismuth ellagate photocatalyst was characterized using several spectroscopic techniques: powder X-ray microscopy (TEM), energy-dispersive X-ray spectroscopy (EDX), thermogravimetric analysis (TGA), Fourier transform infrared spectroscopy (FTIR), and nitrogen sorption measurements. Product formation was confirmed using H-1-NMR, (CNMR)-C-13, and FTIR. The photocatalytic performance of Bi-ellagate was studied for the first time, which exhibits a band gap value of 2.62 eV, endowing it with a high photocatalytic activity under visible light irradiation. The reaction product, N,Nbenzylidenebenzylamine, was selectively obtained with a high conversion yield of similar to 96% under solvent-free conditions compared to other control experiments. The Bi-ellagate photocatalyst was recovered and reused four times without any significant loss in its activity, which provides an eco-friendly, low-cost, recyclable, and efficient photocatalyst for potential photocatalytic applications.