Understanding nanocomposite interfacial bonding under environmental conditions will lead to gamechanging material applications in energy, aerospace, electronics, and infrastructure applications. Carbon nanotube (CNT) yarns with high-temperature toughened matrices are candidates to be used in aircraft and space components. While operating, these components are exposed to severe temperatures, which alter their performance due to changes near the interfacial area. This study investigates the interfacial shear strength of CNT yarns in multiple matrices from near-cryogenic temperatures up to temperatures above the matrix glass transition temperature. Statistical and data-driven approaches are implemented to understand and quantify the interface between inclusion and matrix. The ber bundle pullout test is performed at a broad temperature range for fundamental studies of composite material interfaces and their bonding properties in extreme environments. Analysis showed that IFSS decreases with increasing temperature, especially at temperatures near the resin's glass transition temperature. It was shown that the work required to pull out the CNT from all polymer matrices was reduced by more than 60% between temperature extremes.