There are provided a honeycomb structure and a method of manufacturing the structure, capable of preventing or reducing generation of CO2 or harmful gas during firing to thereby prevent or inhibit pollution and global warming, and capable of obtaining a honeycomb structure having few defects such as cracks and maintaining high strength and low thermal expansion. In a method of manufacturing a honeycomb structure, in which a forming material containing a cordierite forming material and an organic binder is kneaded and formed to prepare a honeycomb-shaped formed article (honeycomb formed article), and the prepared honeycomb formed article is fired to obtain a honeycomb-shaped structure (honeycomb structure) mainly composed of cordierite: the forming material containing a layered clay mineral whose layer charge (X) is 0.2