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Abstract Thin film electronic devices based on flexible biocompatible substrates are desired in various fields such as implants, soft robotics, and wearables, where stretchability is often necessary. Structure‐enabled stretchability in flexible thin films can be achieved by introducing origami‐inspired folds, thereby storing excess material in the out‐of‐plane direction to unfold upon stress. When using vapor‐deposited substrates such as parylene‐C, folds can be introduced prefabrication using molds patterned in repeated grooves and ridges. Here, this work reports the fabrication and parametrization of 10‐µm‐thick stretchable origami parylene‐C electrodes using 3D printed molds. The molds are printed with a sinusoidal pattern and tunable amplitude and slope, with accurate printing results up to 60° steepness. A 160‐nm‐thick gold layer on top of the folded parylene is patterned via laser ablation following the 3D mold shape. Depending on the design parameters, the resulting electrodes maintain functionality until 40%–100% strain. By 3D printing the molds, this technique can fabricate electrodes with complete control of the designed directions of stretchability in a rapid prototyping approach.