Enhancing the durability and functionality of existing materials through sustainable pathways and appropriate structural design represents a time-and costeffective strategy for the development of advanced wearable devices. Herein, a facile graphene oxide (GO) modification method via the hydroxyl-yne click reaction is present for the first time. By the click coupling between propiolate esters and hydroxyl groups on GO under mild conditions, various functional molecules are successfully grafted onto the GO. The modified GO is characterized by FTIR, XRD, TGA, XPS, and contact angle, proving significantly improved dispersibility in various solvents. Besides the high efficiency, high selectivity, and mild reaction conditions, this method is highly practical and accessible, avoiding the need for prefunctionalizations, metals, or toxic reagents. Subsequently, a rGO-PDMS sponge-based piezoresistive sensor developed by modified GO-P2 as the sensitive material exhibits impressive performance: high sensitivity (335 kPa −1 , 0.8−150 kPa), wide linear range (>500 kPa), low detection limit (0.8 kPa), and long-lasting durability (>5000 cycles). Various practical applications have been demonstrated, including body joint movement recognition and real-time monitoring of subtle movements. These results prove the practicality of the methodology and make the rGO-PDMS sponge-based pressure sensor a real candidate for a wide array of wearable applications.