Zn : Al layered double hydroxide-supported 3-aminopropyltriethoxysilane (APTES) and N-methyl 3-aminopropyltriethoxy silane (MAPTES) are found to be efficient, environmentally attractive and selective solid base catalysts for liquid phase aldol condensation reactions at room temperature. The organic functionalized solid catalysts were characterized by XRD, FT-IR, Raman, EDX, SEM, TG-DTA, ¹³C and ²⁹Si CP MAS NMR techniques. The XRD pattern indicated the anti-parallel monolayer arrangements of organic moieties in the interlayer space of LDH. ²⁹Si NMR confirmed that the linking silicon atom is fully condensed in the framework. The reusability study shows consistent activity of the heterogeneous catalyst after several cycles.