Radioisotope thermoelectric generators (RTGs) are deal energy supply devices for deep space and deep-sea exploration, and it is also the energy core of the operation of the working equipment. Except for 238Pu (Plutonium), 241Am (Americium) was also used as a nuclide in the radioactive energy system for future space exploration missions. In this work, neodymium oxide (Nd2O3) was used as analogues for Am2O3. Cold-press-and-sinter methods was used. Different particle parameters (morphology, size, and crystal structure) and synthesized parameters of Nd2O3 were investigated. The synthesized powders contained lath-shaped particles, and batches with different particle sizes and microscopic topography were made and sintered. The results show that the optimal precipitation temperature of Nd2O3 is 25 °C. The optimal thermal decomposition temperature range is 900 °C to 1100 °C, and the optimal thermal decomposition heating rate is 10 °C min−1. The samples of Nd2O3 pellets without cracking is obtained with relative density of 85%–90 %. The Vickers hardness of Nd2O3 pellets was also studied. This paper provides an important scientific guiding significance for the cold-press-and-sinter of radioisotope 241Am batteries in the future.