This paper reports preparation, characterization of amine modified mesoporous crystalline MCM-41 and its application in Knoevenagel condensation reaction. Amine modified MCM-41 was prepared by cocondensation and post-synthesis methods. The samples were characterized by X-ray powder diffraction, Fourier-transfer infrared spectroscopy (FTIR), thermo gravimetric analysis (TGA), differential thermal analysis (DTA), scanning electron micrograph (SEM), Si-29 magic-angle spinning (MAS), nuclear magnetic resonance (NMR), diffuse reflectance spectra (DRS), nitrogen adsorption-desorption and CHN analysis. X-ray diffraction patterns indicate that the modified materials retain the standard MCM-41 structure. SEM study exhibits that the arrangement of particles for 12.8% amine modified MCM-41 is well ordered and spherical in nature. CHN analysis supports that complete hydrolysis of ethoxy groups take place in 12.8% amine modified sample. From the NMR study it is confirmed that the Surface coverage is 40% in 12.8% amine modified sample. The base catalytic activity of hybrid MCM-41 materials Such as amine (post-synthesis and co-condensation methods) and surfactant functionalized materials for condensation reaction between benzaldehyde and diethyl malonate in solvent free. room temperature synthesis of cinnamic acid was evaluated and correlated with the surface and textural properties. Sample containing 12.8 wt% amine loaded by co-condensation method showed highest malonic ester conversion (92%) and selectivity (98%) for cinnamic acid. (C) 2009 Elsevier B.V. All rights reserved.