Cs2CdI4 crystals are grown from the melt (A) and from water solution (B). Optic, dielectric, X‐ray, and calorimetric investigations are carried out. Crystal A shows three phase transitions at 332.3, 259.6, and 183.4 K with following sequence of phases: commensurate orthorhombic of β‐K2SO4 type (a0 = 1.074, b0 = 0.8458, c = 1.4852 nm) ↔ incommensurate ↔ monoclinic ferroelastic (P21n) ↔ triclinic ferroelastic (P1). The B‐crystal belongs to monocline symmetry (P21/m) and undergoes transformation into the orthorhombic phase of β‐K2SO4 type at ≈ 420 K.
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