Many useful clay minerals are not available in sufficient quantities in nature. Actually, two major problems are encountered in the uses of clay minerals, (i) the depletion of the natural deposits, especially those with easy access for mining and (ii) the occurrence as mixtures of several phases. To overcome these problems, laboratory syntheses of clay minerals recently attracted particular interest of scientists in the fields of material science, geology, chemistry, and geochemistry. This chapter provides a comprehensive survey on the synthesis of different clay minerals such as kaolinites, montmorillonites, beidellites, hectorites (Laponite) including the direct synthesis of organohectorites, saponites, and chlorites. Also reported is the technique to hydrothermally synthesize clay minerals with direct incorporation of diverse organic groups. A recent development is the one-step synthesis of layered inorganic-organic materials resembling the parent talc structure.