The organic-inorganic hybrid catalyst was prepared by immobilizing 3-methylaminopropyl moiety onto mesoporous silica, MCM-41, and applied for solid base catalyst of three-component one-pot reaction, i.e. Knoevenagel condensation of aldehyde with the active methylene compound to yield an electron deficient alkene which is subjective to be reacted with nitromethane by Michael addition to form tri-substituted primary nitro compound. The catalyst was characterized by powder-XRD, TG-DTA, FT-IR, nitrogen adsorption-desorption measurement and solid-state cross polarization magic angle spinning (CP/MAS) NMR, and exhibited high catalytic activity in three-component one-pot reaction; however, with poor reusability. (C) 2012 Elsevier B.V. All rights reserved.