Composites of organic compounds and inorganic nanomaterials provide novel sensing platforms for high-performance sensor applications. The combination of the attractive functionalities of nanomaterials with polymers as an organic matrix offers promising materials with tunable electrical, mechanical, and chemisensitive properties. This review mainly focuses on nanocarbon/polymer composites as chemiresistors. We first describe the structure and properties of carbon nanofillers as reinforcement agents used in the manufacture of polymer composites and the sensing mechanism of developed nanocomposites as chemiresistors. Then, the design and synthesizing methods of polymer composites based on carbon nanofillers are discussed. The electrical conductivity, mechanical properties, and the applications of different nanocarbon/polymer composites for the detection of different analytes are reviewed. Lastly, challenges and the future vision for applications of such nanocomposites are described.