The novel organic-inorganic nanocomposites were synthesized via in-situ polymerization of polyaniline (PANI) with mesoporous silica (MCM-41) for methylene blue (MB) dye degradation under visible light. The synthesized PANI/MCM-41 nanocomposites were characterized through Fourier transform infrared (FTIR), X-ray diffraction (XRD), Raman spectroscopy, field emission scanning electron microscopy (FESEM), and UV-visible studies. The structural and optical properties confirmed the interaction between PANI and MCM-41. The photocatalytic experiments showed that the MB dye was efficiently degraded by approximately 70% under light irradiation over the surface of the PANI/MCM-41 nanocomposites. The degradation might occur due to the efficient charge separation of the e(-)-h+ pairs at the interface of PANI and MCM-41 in the excited state under light irradiation.