High-performance polymeric composites are currently being considered as state-of-the-art material systems for future supersonic aircraft and space structures. However, the long-term durability and environmental stability of these materials continue to be under question. Continued application of these composites in aerospace structures is contingent upon the long-term durability of these material systems. Polymeric materials have been known to undergo both physical as well as chemical aging. The aging time, temperature, and environment play a significant role in affecting the physical and chemical aging behavior in the polymers. Currently, there is a dearth of information on the combined effects of physical and chemical aging in polymer-based composites. This study describes the effect of sub-T_g environmental aging on the mechanical properties of two high-performance polymeric composite systems. The effect of chemical degradation on the durability of the material systems is discussed. Further, the effect of environmental stress cracking (ESC) behavior of high-performance composite materials in the presence of organic solvents is investigated and the implications of ESC on durability are studied. Also included in this thesis is a study of the physical aging characteristics of the composites, via measurement of the viscoelastic (creep) properties. Accelerated characterization techniques were employed to predict long-term physical aging behavior. Fiberite 954-2 (a thermoplastic toughened cyanate ester resin) and its graphite-reinforced composites, and Fiberite ITX (a semicrystalline thermoplastic resin) and its graphite fiber-reinforced composites (IM8/ITX) were used in the study. These material systems were under consideration for usage in high-speed civil transport (HSCT) aircraft. This aircraft is expected to have an operating temperature of around 150°C (based on a 2.4 Mach number), an operating pressure at service altitude of 2 psi (0.136 atm), and a flight life in the excess of 60,000 hours at the above-mentioned conditions. The aging of the specimens was carried out for periods of up to 9 months at temperatures between 140°C to 200°C in three different environments; an inert nitrogen environment, an environment with a reduced air pressure of 2 psi (0.136 atm), and ambient atmospheric air. The results from stress-strain, flexure, and micro-indentation tests indicated a substantial reduction in material properties with aging in the different environments. The bending strength, strain to failure, and hardness values of the two composite systems decreased by as much as 20-50%. Tensile modulus on the other hand showed an increase of 20% after 6 months of aging in air, indicating apparent embrittlement with aging. Chemical degradation/damage was also monitored by penetrant enhanced x- radiography, scanning electron microscopy (SEM), and scanning acoustic microscopy (SAM). The chemical aging/degradation was seen to be sensitive to the oxygen partial pressure in the aging environment. The greater the amount of oxygen in the aging environment, the more the loss in the material properties. The glass transition temperatures (T​​_g) of the two material systems were sensitive to both the aging environment and aging time. The T_g of both systems increased over long aging times as seen from dynamic mechanical analysis (DMA) measurements. However, increased oxygen concentrations appear to reduce the T_g. Changes in the T_g of both material systems were a complex behavior attributable to the varying oxygen concentrations in the aging environments, and the combined occurrence of physical aging, degradation, etc. in the materials. The chemical degradation in the composites appears to be via an oxidation mechanism and the micro-indentation results further indicate diffusion-controlled oxidation. Weight changes of samples (neat resin and composites) were also monitored over the entire period of the study and these showed a sensitivity to the oxygen concentration in the aging environment. The greater the oxygen in the environment, the greater the weight loss in the specimens, indicating an oxidation phenomenon. DMA and tensile creep were performed to study the interaction of creep and physical aging in these material systems. Long-term creep predictions of the composites were made using Time-Temperature Superposition (TTSP) and Effective Time Theory (ETT) techniques. The IM8/954-2 composites behaved in an anomalous fashion at times. This may be attributable to the blended nature of the 954-2 resin system, possible post-curing and phase separation of the resin, and thermal decomposition at elevated temperatures. The solvent testing of composites based on thermoplastic polymers revealed susceptibility to ESC. Bending strength losses up to 30% were seen from flexure tests on unidirectional composites. It was also seen that residual stresses in cross-ply laminates were sufficient to trigger ESC after exposure to common organic solvents for an hour. The damage/failure modes were captured by SEM micrographs. / Master of Science