The thermoplastic nature of Parylene C is leveraged to enable the formation of three-dimensional structures using a thermal forming (thermoforming) technique. Thermoforming involves the heating of Parylene films above its glass transition temperature while they are physically confined in the final desired conformation. Micro and macro scale three-dimensional structures composed of Parylene thin films were developed using the thermoforming process, and the resulting chemical and mechanical changes to the films were characterized. No large changes to the surface and bulk chemistries of the polymer were observed following the thermoforming process conducted in vacuum. Heat treated structures exhibited increased stiffness by a maximum of 37% depending on the treatment temperature, due to an increase in crystallinity of the Parylene polymer. This study revealed important property changes resulting from the process, namely (1) the development of high strains in thermoformed areas of small radii of curvature (30-90 µm) and (2) ∼1.5% bulk material shrinkage in thermoformed multilayered Parylene-Parylene and Parylene-metal-Parylene films. Thermoforming is a simple process whereby three-dimensional structures can be achieved from Parylene C-based thin film structures with tunable mechanical properties as a function of treatment temperature.