A method has been developed to synthesize organo-hectorite clays directly from a Mg-silicate gel containing organic or organometallic molecules that are expected to be incorporated within the interlayer space. Complete crystallization occurs upon aqueous reflux for 48 h. The progress of clay layer formation was monitored by X-ray powder diffraction (XRD), differential thermal gravimetry (DTG), and infrared (IR) spectroscopy. Evidence of clay XRD peaks occurs after just 4 h of hydrothermal treatment, and Mg(OH) 2 is no longer observable after 14 h. Observable changes in DTG and IR occur at about this time as well. Warren line-shape analysis of the 110 reflection indicates that when growth is complete the clay lamellae are on average approximately 50% and 25% of the size of natural hectorites and montmorillonites, respectively. The N 2 BET surface areas for all materials are also compared. Small angle neutron scattering shows that addition of tetraethyl ammonium (TEA) ions does not alter the structural integrity over that of the purely inorganic form of Li-hectorite, but that use of a cationic polymer does significantly alter the microstructure. The effect of temperature is critical, for at room temperature only the layered Mg hydroxide mineral brucite crystallizes unless very long time scales are used. The crystallizations carried out at room temperature show that clay will form after about 3 months, but that the presence of organics (at least TEA) acts to hinder this process greatly. The role of the organic molecules on silicate clay layer formation is compared with the role of organics in zeolite synthesis.