Morphotropic phase transitions take place in NdAlO3−TbAlO3 and NdAlO3−DyAlO3 systems. Lattice parameter crossover occurs in Nd1−xTbxAlO3 and Nd1−xDyxAlO3 solid solutions. Temperature-induced phase transition Pbnm↔R 3¯≿ has been detected in both systems. Phase diagrams of the NdAlO3−TbAlO3 and NdAlO3−DyAlO3 systems have been constructed.