Synthesis of large-area patterned MoS 2 is considered the principle base for realizing high-performance MoS 2 -based flexible electronic devices. Patterning and transferring MoS 2 films to target flexible substrates, however, require conventional multi-step photolithography patterning and transferring process, despite tremendous progress in the facilitation of practical applications. Herein, an approach to directly synthesize large-scale MoS 2 patterns that combines inkjet printing and thermal annealing is reported. An optimal precursor ink is prepared that can deposit arbitrary patterns on polyimide films. By introducing a gas atmosphere of argon/hydrogen (Ar/H 2 ), thermal treatment at 350 °C enables an in situ decomposition and crystallization in the patterned precursors and, consequently, results in the formation of MoS 2 . Without complicated processes, patterned MoS 2 is obtained directly on polymer substrate, exhibiting superior mechanical flexibility and durability (≈2% variation in resistance over 10,000 bending cycles), as well as excellent chemical stability, which is attributed to the generated continuous and thin microstructures, as well as their strong adhesion with the substrate. As a step further, this approach is employed to manufacture various flexible sensing devices that are insensitive to body motions and moisture, including temperature sensors and biopotential sensing systems for real-time, continuously monitoring skin temperature, electrocardiography, and electromyography signals.