Nano-sized BaNd2Ti5O14 powders were prepared by the spray pyrolysis process. Sucrose used as the organic additive enabled the formation of nano-sized BaNd2Ti5O14 powders. The powders prepared from the spray solution without sucrose had a spherical shape, dense structure and micron size before and after calcination. However, the precursor powders prepared from the spray solution with sucrose had a large size, and hollow and porous morphology. The precursor powders had an amorphous crystal structure because of the short residence time of the powders inside the hot wall reactor. The complete decomposition of sucrose did not occur inside the hot wall reactor. Therefore, the precursor powders obtained from the spray solution with sucrose of 0.5M had a carbon content of 39.2wt.%. The powders obtained from the spray solution with sucrose of 0.5M had a slightly aggregated structure of nano-sized primary powders of BaNd2Ti5O14 crystalline phase after calcination at 1000˚C. The calcined powders turned into nano-sized BaNd2Ti5O14 powders after milling. The mean size of the BaNd2Ti5O14 powders was 125 nm.