Different amine-functionalized mesoporous zirconia were prepared by a co-condensation method using silane [aminopropyltrimethoxysilane (APTES), N-(2 amino ethyl)-3-amino propyl trimethoxy silane (AAPTMS), and 3-[2-(2-amino ethyl amino) ethyl amino] propyl trimethoxy silane (AEPTMS)] and zirconium butoxide. The materials were characterized by X-ray diffraction, BET surface area analysis, C-13 magic angle spinning-nuclear magnetic resonance (NMR), Fourier transfer infrared spectroscopy (FTIR), scanning electron micrography (SEM), and thermogravimetric analysis (TGA)-differential thermal analysis (DTA). FTIR and NMR results revealed the successful grafting of organic amines onto the surface of zirconia. The catalytic activities were investigated for liquid phase Henry reaction of aromatic aldehydes with nitro methane.