From healthcare to environmental sensors, small operational devices are being developed to monitor and report in a host of new environments. These varied environments require widely varying material properties to meet operational challenges. Unfortunately, the tools used for device fabrication are not fully compatible with the breadth of substrates being utilized. The ability to transfer operational devices from a fabrication‐friendly substrate to any arbitrary substrate is essential to meet needs. Single layer hydrogenated graphene (HG) is an excellent candidate to support the transfer of operational devices. Hydrogenation of graphene weakens the film's van der Waals interaction with its substrate, allowing it to delaminate in water. The free‐floating HG layer can then be placed onto a new substrate. In this work, this property is exploited to transfer working field‐effect transistors (FETs) and gas‐sensing polymer films onto representative hard and flexible substrates. The transferred devices are operational in place and are spaced only one atomic layer away from their final substrate surface. The versatility of HG‐assisted device transfer is also demonstrated by transferring devices onto curved, irregular, and fragile surfaces that are otherwise not fabrication‐friendly, including an nuclear magnetic resonance (NMR) spectroscopy tube, plastic water bottle, waxy plant leaf, and a culture of live neurons. [ABSTRACT FROM AUTHOR]