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Due to the fast development of human culture, environmental issues including water pollution, air pollution, and natural resources abuse present severe impacts on human life. The development of versatile and personal use sensors has become one of the most popular ways to improve personal protection from exposures to different types of environmental threats. The ultra-high-specific surface area and porosity of micromaterials or nanomaterials, and the easy operation of color signals make nanofibrous membrane-based colorimetric sensors highly attractive in sensitively monitoring environmental toxicants. In this chapter, we highlight recent progresses in developments of colorimetric sensors, which are mainly based on the use of nanofibrous membranes for toxic vapors by taking its merits of ultra-high specific surface areas, light weight, and flexibility. Different sensors targeting on volatile organic compounds, vaporous pesticides, volatile nerve agents, and corrosive gases are included. It is expected to provide guidance for the development of colorimetric sensors not only present remarkable sensitivity and selectivity but also are suitable to be embedded into the next generation of smart textiles.