Nanocomposites of SiO2/MoO3 having respective weight ratios of 3:1, 2:2, and 1:3 were synthesized using a nanosecond pulsed laser ablation method. The prepared samples were analyzed with UV-Vis and Raman spectroscopy, XRD, SEM, EDX, and TEM. Based on the TEM analysis, the morphology and the structure of the nanocomposites varied with the change in the ratio of MoO3, and the sample containing the highest amount of MoO3 shows a compact morphology and a higher number of nanoparticles. The band gap energy of the nanocomposites increases with an increase in MoO3 load. The nanocomposites were used in the catalytic reduction of 4-nitrophenol (4-NP) in the presence of NaBH4. The reduction time of 4-NP decreases as the amount of MoO3 increases in the nanocomposite. The rate constants were estimated at 0.0878, 0.2319, and 0.1726 min-1 for SiO2/MoO3 (3:1, 2:2, and 1:3) catalysts respectively. The results demonstrate the good catalytic performance of the prepared materials by enabling fast reduction of 4-NP.