Both 3D organic-inorganic perovskites ([Et3P(CH2)2Cl][Cd(dca)3] (1) and [Et3P(CH2)2F][Cd(dca)3] (2) [dca = dicyanamide, N(CN)2-]) display two sequentially reversible high-temperature phase transitions and switchable dielectric properties. Through halogen substitution, 1 shows exceptional switching behaviour of second harmonic generation effects and remarkably 2 represents the first above-room-temperature 3D ferroelastic material characterized by two ferroelastic phases.