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Modern medical treatment techniques widely employ principles of theranostics using non-invasive diagnostics modalities. Optical diagnostics techniques have high potential here owing to high spatial resolution and ultimate functional capabilities. Nanosized agents open wide prospects in developing theranostics approaches assisted by optical imaging due to advanced technologies for fabricating nanoproducts with customized properties. Many classes of nanoproducts, however, exhibit significant toxicity, which limits their application in biomedical studies. Silicon nanoparticles are a perspective class of theranostics agents due to their biocompatibility and biodegradability and unique optical properties. In this report we tell about a novel dual-stage technique for fabricating silicon nanoparticles that are promising for optical theranostics. The principle of the developed approach consists in fabrication of porous silicon films or silicon nanowires arrays with reduced laser ablation thresholds followed by high-yield generation of nanoparticles by means of laser ablation in liquids at second stage. A comprehensive study of structural and optical properties of produced nanoparticles is reported together with pilot results of visualization with optical coherence tomography and fluorescence imaging.