Silica sol-gel entrapped acids, bases and organometallic catalysts are used successfully in one-pot reactions without interfering with each other. Both physically and covalently entrapped acids and bases were employed in these processes, including polystyrene sulfonic acid, 1-propane sulfonic acid, molybdosilicic acid (SiO2-MoO3), poly[(vinylbenzyltrimethyl)ammonium] hydroxide and 1,5,7-triazabicyclo[4.4.0]decene. The entrapped metal-based catalysts are Rh2Co2(CO)12 and RuCl2(PPh3)3. The one-pot reactions carried out with these heterogenized reagents and catalysts include formation of alkenes under acidic and basic conditions, C—C bond formation by condensation reactions with an α-carbon to a carbonyl, hydroformylation and hydrogenation.