In the current paper, a NiO nanoparticles-loaded mesoporous carbon (CMK-3) catalyst, denoted as NiO/CMK-3, has been successfully synthesized using a facile strategy. The as-prepared material has been characterized through XRD, Raman spectroscopy, low-temperature N2 physisorption measurements, FTIR, FE-SEM, TEM, and XPS. The as-fabricated NiO/CMK-3 catalyst manifested a superior activity in the NaBH4-assisted reduction of methylene blue (MB) dye to its colorless leuco form. Remarkably, over 99% of 25 mg L−1 MB was reduced by 7.5 mM/L NaBH4 using 0.1 g L−1 NiO/CMK-3 within 3 min at room temperature. Furthermore, the kinetics study confirmed the appropriateness of the pseudo-first-order kinetic model for elucidating the kinetics of MB reduction by the catalyst. Importantly, the NiO/CMK-3 catalyst maintained almost constant catalytic activity even after 5 times of reuse in MB reduction, demonstrating its superior stability and reusable ability. So, NiO/CMK-5 appears as a promising heterogeneous catalyst for the effective remediation of dye-containing wastewater.