jats:titleAbstract</jats:title>jats:pModern electronic devices, particularly those intended for wearable or human health monitoring applications, require high levels of flexibility and stretchability. Hence devices, as well as interconnects, need to be capable of retaining functionality even when being mechanically deformed. Most approaches towards achieving this rely on printing or transferring structures onto elastomeric substrates that can withstand stretching. However, the processing involved can often be cumbersome, and the structures themselves tend to suffer from poor fatigue and/or are limited by the mechanical properties of the underlying substrate. Here, we have developed a novel aerosol jet printing technique capable of building fully freestanding functional structures layer by layer, which are robust and reliable upon thousands of stretching cycles. The process involves printing a combination of layers of different materials with the desired functionality, onto a substrate coated with a sacrificial film that is subsequently dissolved to release the printed structure. Using this method, we demonstrate freestanding conductive wires that can be used as stretchable interconnects/electrodes, and that also function as strain‐sensors. Additionally, we show that a freestanding capacitive structure functions as a robust, stretchable humidity sensor, paving the way for the development of other multilayer, multifunctional stretchable devices and sensors.</jats:p>