Methods for rapid, safe and effective detection of unmapped buried ordnance are vital to the protection of humans and environmental quality throughout the world. This study aimed to investigate the use of phytosensing and to understand the physiological response of woody plants to 2,4,6-trinitrotoluene (TNT) contamination. Baccharis halimifolia were potted in soils containing various concentrations of TNT and physiological responses were observed over a 9-week experimental period. Measurements included the collection of remotely sensed data, such as hyperspectral reflectance and chlorophyll fluorescence, and traditional plant-level physiological data. In accordance with the hypothesis, low levels of TNT improved physiological response in plants due to the slight increase in nitrogen, while high levels of TNT induced stress. Key markers in stress responses were identified, specifically with reflectance indices and derivatives, which may separate TNT-contaminated plants from naturally stressed plants and would allow for accurate detection of buried ordnance at the landscape level.