Synthesis temperature and purity of core/shell nanocrystals are key challenges facing the scientific community. Moreover, the core/shell structures usually need a multi-step synthesis pathway to be fabricated. This work aims to address these challenges by developing an innovative one-step synthesis pathway for obtaining carbonate-free BaTiO 3 core/shell nanocrystals at low temperature. The results show that very fine BaTiO 3 core/shell nanocrystals (<11 nm) free from any by-products such as BaTi 2 O 5 and BaCO 3 are synthesized at 323 K (50 °C). This newly developed structure can significantly reduce the sintering temperature of the nanocrystals and can be beneficial in fabricating the ceramic parts at lower sintering temperatures. 3 significantly change its dielectric behavior and turn dielectric nature of BTO to semiconducting one [21].Facile strategies for nanocrystals synthesis are of fundamental importance in the advancement of nanoscience and nanotechnology. In this work, it has been tried to develop and describe a new methodology for the synthesis of carbonate-free BTO nanocrystals. This methodology provides a one-step, convenient, low-cost, nontoxic, and mass-productive route for the synthesis of BTO nanocrystals. On the other hand, BTO is conventionally obtained by solidstate synthesis between barium carbonate (BaCO 3 ) and titania (TiO 2 ) at 1473 K (1200°C) [18][19]. Some wet chemical approaches need a calcination process at temperatures above 973 K (700°C) [11]. The products of these methods contain some inhomogenities and by-products [13,16]. As the great advance made by this work, our method of synthesis is able to obtain high-quality homogenous carbonate-free BTO nanocrystals at a low temperature of 323 K (50 °C).Core-shell nanostructures have recently received much attention for their enhanced properties and performances [24][25][26][27]. Moreover, the core-shell structures are normally chosen believing that these can cause a better coupling between the two phases. In this work, a new family of core-shell structure is developed which the core and shell have similar composition while core are crystalline and shell is amorphous. Moreover, for the first time, the novel core/shell nanostructures are obtained by a one-step synthesis method. On theother hand, obtaining nanocrystalline ceramic parts from their nanopowders is one of the most important challenges facing the scientific communities since the high temperature of the sintering process results in particle growth and as the consequence; the final structure becomes submicron-sized. When the shell is amorphous, this layer absorbs thermal energy to become crystalline and thus the required energy for particle growth cannot be provided. TheIn stage (i), the decarbonation treatments of deionized water are performed in three stages including boiling at 373 K (100 °C) for 30 min, bubbling with Ar gas for 30 min and increasing the pH of deionized water above pH 8.5. This three-stage process leads to removal of the carbon species and dissolved CO 2 gas fr...