The tunable mechanical and stretchable properties of thermoplastic polyurethane (TPU), in conjunction with its convenience of surface modification, have attracted interest for various sensing materials. This study examines the process of creating conductive and flexible TPU composites by incorporating carbon materials such as graphene oxide (GO) and polypyrrole (PPy). The suitability of these composites for ammonia gas sensing and as supercapacitor electrode materials is investigated for evaluating the potential of the dual-functioning hybrid composites. Two fabrication process sequences are examined: one involves surrounding TPU with GO and subsequently adding PPy, and the other involves wrapping TPU with PPy and incorporating GO. The results reveal that the fabrication process sequence can be adapted to control the mechanical and electrical properties of TPU composites. Furthermore, the conductive TPU composites exhibit significant potential for dual-function applications as both ammonia gas sensors and supercapacitor electrode materials. Among the TPU composites tested, TPU-PPy-GO demonstrates the best performance in terms of gas sensing and supercapacitor capabilities. A further evaluation of TPU-PPy-GO focuses on its selectivity and sensitivity to other reducing gases (triethylamine, ethanol, and methanol) and its galvanostatic charge−discharge properties for energy-storage electrode applications. By modification of the fabrication sequence, conductive TPU composites can be used extensively as chemical sensors and energy storage materials.