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Surrounding air pollution is one of the important warnings to human health. It is necessary to detect hazardous pollutant gases in the air. The gas sensor is the candidate for such detection. Progress of smart and flexible sensors has been receiving growing curiosity in recent years because of their enormous sensing applications. Such smart and flexible sensors can be manufactured by depositing conducting materials, such as conducting polymer, carbon nanotube (CNT), graphene oxide, and metallic nanoparticles, onto nonconducting polymeric flexible substrates, such as paper, plastic films, and textiles. Most of the flexible polymeric substrates, such as polyethylene, polyester, nylon, and polypropylene, have low surface energy and poor wettability, which weakens the adhesion between conducting material and flexible substrate. Plasma surface modification is a novel technique to enhance surface properties to produce stable composites. This review focuses on various types of plasmas for surface modification and their effects on the surface after plasma treatment to improve the grafting and adhesion of the sensing layer with the substrate. The aim of this article is to systematically overview the development of plasma-enhanced smart and flexible gas sensors to date and to envisage their future progress. [ABSTRACT FROM AUTHOR]