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This paper discusses a modified sol–gel process, which can prepare nanocrystalline BaTiO3 powders, fibers, and thin films. This process involved the preparation of stable precursor solutions containing the respective aqueous acetate solution of barium acetate and titanium isopropoxide where barium acetate and titanium isopropoxides were used as precursors and aqueous acetic acid was used as a solvent. The gel prepared using this precursor solution was calcined at 550°C/2 h to produce nanocrystalline BaTiO3 with the corresponding average X-ray particle size of ∼15 nm. In case of thin film, precursor solution was directly deposited on silicon or glass substrates by spin coating. Nanocrystalline BaTiO3 powders were dispersed into the precursor solution to produce a thick, crack-free particle film. We have also prepared BaTiO3 fibers by soaking plant fiber (Jute) in the precursor solution. Heat treatment of soaked and dried plant fiber produces BaTiO3 fibers. Particle, fiber, and film surfaces were characterized by transmission electron micrograph and scanning electron micrograph analysis. Altogether, this is a new direction for the development of multiple structures from the same precursor solution.