Wireless, skin‐interfaced electronic and microfluidic devices have the potential to replace wired, bulky, and cumbersome technologies for personal and clinical health monitoring, allowing care to extend from hospital settings to the home. For use on skin, these devices commonly employ silicone‐based thermoset elastomers (TSEs) as layers that encapsulate the electronics or serve as molded microchannels for biofluid (e.g., sweat) capture, storage, and analysis. Barriers to commercial adoption of such devices include difficulties in use of these elastomers in conventional practices for mass manufacturing. Their relatively high cost and inability to allow for recycling represent additional disadvantages. By contrast, thermoplastic elastomers (TPEs) are fully compatible with industrial‐scale manufacturing processes, low in cost, and recyclable. Like TSEs, TPEs are soft, stretchable, flexible, and optically transparent, while possessing other properties well‐suited for applications in wireless, skin‐interfaced devices. Herein, the characteristics, processing, and application techniques for three commercially available TPEs, including two thermoplastic polyurethanes as encapsulation layers for a wireless skin hydration sensor and one thermoplastic styrenic block copolymer for a microfluidic sweat analysis platform, are reported. The results demonstrate that TPEs can be effectively integrated into these classes of devices, as a compelling alternative to TSEs, as a mass‐manufacturable, sustainable materials option.