For the first time to the best of our knowledge, CeAlO3 nanocrystals with perovskite structure are synthesized by pulsed laser ablation technique. The morphological and optical properties of the obtained CeAlO3 nanocrystals are investigated. This work opens new prospects for the application of laser ablation methods for the generation of perovskite nanocrystals and development of novel nanocomposite structures, which can be applied for the fabrication of perovskite solar cells, scintillation detectors, catalysts, etc.