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Zeolite and molecular sieve syntheses are reviewed. The synthesis of aluminum-rich zeolites, high-silica zeolites, and phosphate-based molecular sieves are evaluated. Unresolved mechanistic issues are outlined, and areas for exploration suggested. The ability to plan zeolite and molecular sieve syntheses is discussed and a strategy for synthesizing a chiral zeolite is used to demonstrate the current limitations in “designing” new molecular sieves.