Magnetic characteristics, magnetocaloric effect, and critical behavior of Nd1−xSrxMnO3 compounds by Sr doping (x = 0.2, 0.3, 0.4, 0.5) were studied. All samples maintained orthorhombic structures, but the space group changed from Pnma (No. 62) for x = 0.2, 0.3 to Imma (No. 74) for x = 0.4, 0.5. As Sr doping increased, the Curie temperature (TC), Curie–Weiss temperature (TCW), and magnetization increased, attributed to the double exchange (DE) interaction. A discrepancy between TCW and TC was observed due to the competition between polarons and DE interaction. The critical behavior was investigated systematically using the self-consistent (modified Arrott plots, MAP) method and the Kouvel–Fisher (KF) relation. The KF relation was suitable for the samples with x = 0.2 and 0.5, while the MAP method was suitable for the samples with x = 0.3 and 0.4. Among the Ising, XY, Heisenberg, and mean-field models, the samples with x = 0.2, 0.3, and 0.4 aligned more closely with the mean-field model, except for the x = 0.5 sample. Entropy change (−ΔSM) of Nd1−xSrxMnO3 (0.2 ≤ x ≤ 0.5) increased with the applied field, with the maximum value observed around TC. For the sample with x = 0.3, (−ΔSM) reached 4.315 J/kg K at μ0ΔH = 50 kOe, corresponding to a relative cooling power (RCP) of 280.48 J/kg. Remarkably, the x = 0.4 sample displayed (−ΔSM) of 3.298 J/kg K at μ0ΔH = 50 kOe near room temperature, with the RCP of 283.64 J/kg. These findings underscore the role of Sr doping in tuning the magnetic properties, critical behavior, and magnetocaloric effect of NdMnO3.