The ability of carbon nanofibers grown on nanoelectrode chips for ultrafast detection of molecules down to parts per billion (ppb) with a response time in seconds and with a minimal usage of power has attracted the attention of materials researchers and nanotechnology explorers-for example, space research organizations. Application in chemical and biological sensing is being studied extensively. NASA in their report on failure of space missions released in 2008 emphasized on the need for studying extreme environmental behavior of futuristic space materials. Very little work has been done to understand the behavior of the nanofibers operating in low-temperature environments. In this paper, vertically aligned carbon nanofibers (VACNFs) have been characterized for their survival in extreme low-temperature environments using a combination of environmental chamber and atomic force microscopy (AFM). Specifically, this paper characterizes through nanoindentation the mechanical properties and dimensional stability of VACNFs operating in low-temperature environments.