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The synthesis of zeolite A and ZK-4 crystals of high purity and well-defined morphology is described. Three procedures are detailed, leading to cubic crystals of zeolite A with chamfered edges (average size 3–5 µm), cubic crystals of ZK-4 with sharp edges (average size 1–2 µm), and nano-sized cubic crystals of zeolite A with slightly rounded edges (size ≤ 1 µm).