BackgroundOrthodontic treatment with transparent aligners is popular with patients. Any alteration of the plastic material, as subjected to the oral environment, could influence the treatment's durability, the aligner's aesthetic appearance, and the patient's safety. PurposeThis study concerns the physicochemical properties of ClearCorrect® aligners before and after intraoral use, focusing on transparency, surface topography, leachable, polymer glass transition temperature, and viscoelastic properties. MethodsAligners were collected after two weeks of intraoral use. Unused samples were obtained from the manufacturers. Transparency was measured by UV–visible spectroscopy. Chemical modifications were studied using infrared and Raman spectroscopies. Thermal degradation, glass transition (Tg), and storage modulus (E') were characterized by thermal analysis (DSC, TGA, DMA). Surface morphology and roughness were studied thanks to SEM and AFM. Aligners were immersed in water-based solutions to identify and quantify organic leachable by HPLC chromatography and trace elements by atomic absorption spectroscopy. ResultsClearCorrect® aligners have a three-layer structure (outer PETG/inner PU layers). Slight chemical alterations occurred after aging. There was also no significant evolution in Tg and thermal degradation temperatures and only a minimal evolution of E'. Surface and transparency alterations occurred. A difference in organic compound and trace element release levels between new and used aligners was evidenced, suggesting an intraoral release during use. SignificanceIntra-oral aging mainly impacts the aligner transparency and surface. The leachable study suggests significant ingestion of organic and non-organic compounds by the patient: investigations are needed to assess the impact of the long-term use of trays on patient health.