It is often desirable to cause rapid thermal cycles in isolated systems, and it is convenient to do so by means of radiant heating and cooling. In principle, the rate of heating is arbitrarily increased simply by applying sufficient irradiance. This is not true for cooling, wherein the radiant emittance of a surface is determined by its emissivity and temperature. In an optically thin structure, the cooling rate is determined by the ratio of the material's emissivity to its specific heat, a factor that is expected to be greater in materials with a short characteristic absorption length, such as graphite. Herein, several forms of carbon‐based nanostructures, which have very short thermal radiation attenuation lengths, and are very robust and can withstand the high temperatures required for substantial Planckian thermal radiant emittance, are examined. Rapid cooling times ranging from about 100 μs to 1 ms are observed in structures cooling from a typical high temperature of 1500 K to a low of roughly half that value. Such rapid extreme thermal cycling of isolated materials provides new opportunities, for both research and potentially practical applications.