A new family of transparent, biocompatible, self-adhesive, and self-healing elastomer has been developed by a convenient and efficient one-pot reaction between poly(acrylic acid) (PAA) and hydroxyl-terminated polydimethylsiloxane (PDMS-OH). The condensation reaction between PAA and PDMS-OH has been confirmed by attenuated total reflection Fourier transform infrared (ATR-FTIR) spectra. The prepared PAA-PDMS elastomers possess robust mechanical strength and strong adhesiveness to human skin, and they have fast self-healing ability at room temperature (in ~10 s with the efficiency of 98%). Specifically, strain sensors were fabricated by assembling PAA-PDMS as packaging layers and polyetherimide-reduced graphene oxide (PEI-rGO) as strain-sensing layers. The PAA-PDMS/PEI-rGO sensors are stably and reliably responsive to slight physical deformations, and they can be attached onto skin directly to monitor the body’s motions. Meanwhile, strain sensors can self-heal quickly and completely, and they can be reused for the motion detecting after shallowly scratching the surface. This work provides new opportunities to manufacture high performance self-adhesive and self-healing materials.