Abstract It is well known that illite-smectite can form from smectite at elevated temperatures in natural and experimental systems. However, the conversion of smectite to illite-smectite is also found in some natural systems that have never been heated. The present experiments show that illite layers can form from smectite by chemical reaction at 35° and 60°C at high solution pH. The rate of this reaction is accelerated by wetting and drying.