Surface‐enhanced Raman scattering (SERS) spectroscopy provides a noninvasive and highly sensitive route for fingerprint and label‐free detection of a wide range of molecules. Recently, flexible SERS has attracted increasingly tremendous research interest due to its unique advantages compared to rigid substrate‐based SERS. Here, the latest advances in flexible substrate‐based SERS diagnostic devices are investigated in‐depth. First, the intriguing prospect of point‐of‐care diagnostics is briefly described, followed by an introduction to the cutting‐edge SERS technique. Then, the focus is moved from conventional rigid substrate‐based SERS to the emerging flexible SERS technique. The main part of this report highlights the recent three categories of flexible SERS substrates, including actively tunable SERS, swab‐sampling strategy, and the in situ SERS detection approach. Furthermore, other promising means of flexible SERS are also introduced. The flexible SERS substrates with low‐cost, batch‐fabrication, and easy‐to‐operate characteristics can be integrated into portable Raman spectroscopes for point‐of‐care diagnostics, which are conceivable to penetrate global markets and households as next‐generation wearable sensors in the near future.

Skin‐inspired wearable devices hold great potentials in the next generation of smart portable electronics owing to their intriguing applications in healthcare monitoring, soft robotics, artificial intelligence, and human–machine interfaces. Despite tremendous research efforts dedicated to judiciously tailoring wearable devices in terms of their thickness, portability, flexibility, bendability as well as stretchability, the emerging Internet of Things demand the skin‐interfaced flexible systems to be endowed with additional functionalities with the capability of mimicking skin‐like perception and beyond. This review covers and highlights the latest advances of burgeoning multifunctional wearable electronics, primarily including versatile multimodal sensor systems, self‐healing material‐based devices, and self‐powered flexible sensors. To render the penetration of human‐interactive devices into global markets and households, economical manufacturing techniques are crucial to achieve large‐scale flexible systems with high‐throughput capability. The booming innovations in this research field will push the scientific community forward and benefit human beings in the near future.

Printable, multifunctional, flexible, health monitoring detachable patch sheets with human motion detection capability.