Abstract 3D printing of conductive polymers is an attractive technique for achieving high flexibility, wearability, and sensing characteristics without geometrical limitations. However, there is an urgent need to integrate printability, conductivity, and sensing capability. Herein, a conductive polymer ink for 3D printing that combines the desirable features of high electrical conductivity, flexible stretchability, and strain‐sensing monitoring is prepared. The ink matrix is polydimethylsiloxane and synergistically enhanced by acetylene carbon black (ACB) and multi‐walled carbon nanotubes (MWCNTs) (silane or un‐silane‐modified). The inks are screened step‐by‐step to explore their printability, rheology, mechanical properties, and electrical performance upon loading. The formation of an electrically conductive network, electrical properties upon tensile load, and strain sensing stability under cyclic stretching are investigated intensively. It is demonstrated that conductive polymers filled by ACB and silane‐modified, MWCNTs (MWCNTs‐MTES) possess superior printability, stretchability, conductivity, and strain sensing behaviors. Finally, a flexible wearable strain‐sensing skin patch is printed, and it successfully records joint motion signals on human fingers, wrists, and elbows with good stability and repeatability. Those results show the extent of potential applications in healthcare and motion monitoring fields. This work provides an efficient and simple route to achieve comfortably wearable and high‐performance strain sensors.
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