The structure and thermal property of organomontmorillonite (OM) were studied by X-ray diffraction (XRD), differential thermal analysis (DTA), and thermalgravimetric analysis (TGA).Based on the thermal property of OM, a new method for quantitative characterization of the alkyl-ammonium adsorbed in the layers was established, and the influence of adsorption amount on the viscosity of OM gel was examined. Changes in the basal spacing of OMs and Na-montmorillonite (Na-mont) indicated that alky-ammonium ions intercalated into the montmorillonite layers. TGA results showed that OM and Na-mont had different thermal property, Na-mont held more free water in the layers. The intercalated alkyl-ammonium in OMs decomposed at the temperature of 230~480°C. Effective dosage (DOSeffective) has significant influence on the viscosity of OM gel. Under the optimal DOSeffective(1.1~1.3CEC), the alkyl-ammonium cations can fully cover the exchangeable site in the layers, then the “card-house” structure formed. Structure of the alkyl-ammonium cations determines the intercalation efficiency, the longer the carbon chain, the higher the intercalation efficiency. The intercalation efficiency has no evident correlativity with the viscosity; however, structure of the alkyl-ammonium cations determines their arrangement in the layers.