The crystal structure, magnetic and magnetostrictive properties of high-pressure synthesized PrxNd1−xFe1.9 (0 ≤ x ≤ 1.0) alloys were studied. The alloys exhibit single cubic Laves phase with MgCu2-type structure. The initial magnetization curve reveals that Pr0.2Nd0.8Fe1.9 has a minimum magnetocrystalline anisotropy at 5 K. The magnetostriction curve at 5 K shows that Pr0.2Nd0.8Fe1.9 has a very good low-field magnetostrictive property, and the magnetostriction of the PrxNd1−xFe1.9 alloy in high magnetic field is attributable mainly to Pr. The temperature dependence of the magnetostriction (λ‖) at the field of 5 kOe shows that the substitution of Nd reduces the K1 remarkably, and the values of λ‖ of Pr0.2Nd0.8Fe1.9 and Pr0.8Nd0.2Fe1.9 alloys are nearly five times larger than that of the PrFe1.9 alloy below 50 K; the λ‖ of Pr0.8Nd0.2Fe1.9 reaches up to 1082 ppm at 100 K, which makes it a potential candidate for application in this temperature range.