An addition polyisoimide prepolymer was modified through the incorporation of metal particles. The response of this metal/polymer composite to mechanical vibrations and the passage of electric current was measured. Model aluminum conductor bar joints containing this material were assembled and exposed to elevated temperatures for extended periods of time while the electrical properties of the composites were monitored. In the most favorable systems, no thermal degradation of the electrical properties was observed. Dynamic mechanical behavior of the metal/polymer composites indicated good adhesion between particles and the matrix and also a broadening of the glass transition region as well as a post Tg dispersion in the temperature spectrum. The adhesive properties of these metal/polymer composites to aluminum were studied and found to be influenced by the loading level of the metal in the composite. Chemical reactions occurring during the cure of a neat resin sample of the polyisoimide prepolymer were monitored using infrared spectrometry and differential scanning calorimetry. Both the crosslinking and isomerization reactions were found to be apparently first order with the isomerization having a lower activation energy than the crosslinking. Linear, high molecular weight, thermoplastic polyimides and poly(imide-siloxane) homo- and copolymers prepared by bulk and solution thermal imidization were investigated as structural adhesives for titanium. The solution thermal imidization procedure was found to result in favorable adhesive characteristics while the presence of siloxane segments in the polymer backbone improved the resistance of stressed specimens to moisture. Aluminum-sec-butoxide used as a primer was also found to improve the moisture durability of bonds prepared with these materials. / Ph. D.