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Clays, especially montmorillonite and bentonite are environmentally benign, recyclable, and economical when used as a catalyst. Heteropoly catalysts are also used in a wide variety and high potential, because of their higher catalytic activity and acidic strength than the mineral acids. By the modification of clays with a variety of HPAs, we can achieve the benefits of using both clay and HPAs. We can use various HPAs such as Silicotungstic acid (STA), Phosphotungstic acid (PTA), Silicomolybdic acid (SMA), Phosphomolybdic acid (PMA) for the modification of clay and may be obtained a series of HPA modified clays. HPA modified clays have proved to be a prominent catalyst for different acid-catalyzed organic reactions.This book represents the basic properties of clays and heteropoly acids and the modification techniques of clays with HPAs. These modified clays further characterized by using analytical, thermal, and spectral techniques and find applications as catalysts in organic reactions.