Extrusion Printing of Surface‐Functionalized Metal‐Organic Framework Inks for a High‐Performance Wearable Volatile Organic Compound Sensor

Abstract Wearable sensors hold immense potential for real‐time and non‐destructive sensing of volatile organic compounds (VOCs), requiring both efficient sensing performance and robust mechanical properties. However, conventional colorimetric sensor arrays, acting as artificial olfactory systems for highly selective VOC profiling, often fail to meet these requirements simultaneously. Here, a high‐performance wearable sensor array for VOC visual detection is proposed by extrusion printing of hybrid inks containing surface‐functionalized sensing materials. Surface‐modified hydrophobic polydimethylsiloxane (PDMS) improves the humidity resistance and VOC sensitivity of PDMS‐coated dye/metal‐organic frameworks (MOFs) composites. It also enhances their dispersion within liquid PDMS matrix, thereby promoting the hybrid liquid as high‐quality extrusion‐printing inks. The inks enable direct and precise printing on diverse substrates, forming a uniform and high particle‐loading (70 wt%) film. The printed film on a flexible PDMS substrate demonstrates satisfactory flexibility and stretchability while retaining excellent sensing performance from dye/MOFs@PDMS particles. Further, the printed sensor array exhibits enhanced sensitivity to sub‐ppm VOC levels, remarkable resistance to high relative humidity (RH) of 90%, and the differentiation ability for eight distinct VOCs. Finally, the wearable sensor proves practical by in situ monitoring of wheat scab‐related VOC biomarkers. This study presents a versatile strategy for designing effective wearable gas sensors with widespread applications.