We present a simple but efficient method to prepare carbon nanotube (CNT)-based flexible devices embedded in polymer substrates. In this strategy, a methyl-terminated self-assembled monolayer is first coated on a solid substrate as a release layer, and CNT-network devices fabricated on it are directly transferred into a poly( dimethylsiloxane) ( PDMS) mold, resulting in flexible CNT-network devices embedded in PDMS. The embedded circuits exhibit stable operation even after significant bending. We also propose Raman spectroscopy as a powerful tool to remotely characterize the CNT-network device structures covered by a polymer layer. As a proof of concept, we demonstrate DNA sensors utilizing the fabricated CNT-network devices.