The influence of the strontium concentration on the structure stability and magnetic properties of Nd1-xSrxMnO3 compositions (x = 0; 0.15; 0.25; 0.50) is investigated. An increase in the strontium concentration causes an averaging of the Mn–O bond lengths, an increasing in the Mn–O–Mn angles of Nd1-xSrxMnO3 compositions and a decreasing by more than 2 times in the temperature of the Jahn-Teller phase transition. The doping of Sr = 0.5 changes in the space group of the crystal structure of the undoped NdMnO3. All studied compositions demonstrate: ferromagnetic ordering, antiferromagnetic ordering in the manganese sublattice, and ordering in the neodymium sublattice. The features of the magnetic behavior are due to a decrease in the Jahn-Teller distortion when doped with strontium at a concentration of x = 0–0.25, and a change in the space group of x = 0.5. Strontium doping increases the ferromagnetic response and the Curie temperature. Nd0.5Sr0.5MnO3 has TC = 240 K and is a promising magnetic material for functional applications.