Perovskite-type Nd1−xLaxCrO3(0 ≤ x ≤1.0) polycrystalline samples were synthesized using solid state reaction. Structural studies indicate that the lattice parameters, metal–oxygen bond lengths, and angles of Nd1−xLaxCrO3 strongly depend on the La content. Two magnetic transition temperatures, Cr3+ antiferromagnetic ordering temperature (TN) and the spin reorientation phase transition temperature (TSRPT), have been observed in the M-T curves. The increase in TN and decrease in TSRPT with increasing x value can be explained by the change in the magnetic interactions due to La doping. The heat capacity of Nd1−xLaxCrO3 measured from 2 to 300 K reveals that the lattice, electronic, and magnetic contributions to heat capacity can be well interpreted quantitatively using the Debye and Schottky models. The splitting energy of the Cr3+ 3dt2g orbital and the Nd3+ ground state have been calculated by fitting to the Schottky anomaly at very low temperature. The Cr–Nd interaction is suppressed gradually by La doping, which is verified by the calculation of the mean-field interaction parameter. This doping dependence provides directed evidence of TM–RE magnetic interactions in perovskite compounds, in agreement with the proposed model.