The unusual low-temperature magnetostrictive property is of fundamental interest due to significant applications in rapidly developing cryogenic engineering. Here, we report a giant isotropic magnetostriction (λ = 1500 ppm, ω = 4500 ppm) over a wide temperature range (∼210 K), and the saturated volume magnetostriction can be up to 8400 ppm in cubic NaZn13-type LaFe13−xAlx compounds by optimizing the chemical composition. The large magnetostrictive effect often occurs in ferromagnetic materials. However, we discovered that the magnetic-field-induced volume expansion originates from the change of lattice parameters across the first-order transition from the low-volume antiferromagnetic ground state to the high-volume ferromagnetic state. Moreover, the magnetostrictive materials show an excellent zero thermal expansion (ZTE) property, which guarantees their reliability and stability operating at various temperatures. The present study suggests potential applications of La(Fe, Al)13-based compounds as ZTE and magnetostrictive dual-function materials in cryogenic engineering.