Flexible electronics greatly facilitate human life due to their convenience and comfortable utilization. Liquid metals are an ideal candidate for flexible devices; however, the high surface tension and poor surface wettability restrict their application on diverse substrates. Herein, a printable and recyclable ink composed of poly(vinyl alcohol) and a liquid metal (PVA-LM) was developed to resolve these problems. The materials were designed considering the compatibility between PVA and the liquid metal, and the composite theory was applied to determine the component proportion. The developed composites improved the surface wettability of the liquid metal on diverse substrates, and three-dimensional (3D) printing technology was chosen to maximize the use of this material. Moreover, the PVA-LM ink showed excellent conductivity of about 1.3 × 105 S/m after being turned on, which favored the designing of alarm systems and object locators. The flexible sensors produced with this ink have broad application, high sensitivity, and superstable signal generation even after 200 cycles. When acting as strain sensors, the constructed composites had high sensitivity for monitoring the human movements. Furthermore, liquid metals in printed products can be recycled under alkaline conditions. This study opens a new direction for the next generation of environmentally friendly flexible devices.