Segmented polyurethaneureas (SPUU) are thermoplastic elastomers with excellent elastic properties, high abrasion resistance and tear strength, making them very useful in numerous industrial applications ranging from microelectronics (slurry pad) to biomedical (artificial heart vessels) applications. The elastic and mechanical properties of these materials are strongly influenced by their two phase morphology. The factors that influence phase separation include difference in polarity between the hard and soft phases, composition and temperature. In general good phase separation results in materials with superior mechanical and elastic properties. Due to the immense potential applications of SPUU elastomers, there is a need for materials with higher strength. However, higher strength is not desired at the detriment of elasticity. If fact, stronger materials with enhanced elasticity are desired. In this thesis, high-strength SPUU elastomers were synthesized by incorporating reactive Laponite particles with surface-active free amine. The synthesis of pure SPUU is very complex, and addition of a reactive silicate further increases the complexity. To remedy this challenge, combinatorial methods and high-throughput screening techniques were used to optimize the diamine concentration and cure temperature. It was determined that pure SPUU elastomers prepared at a diamine stoichiometry of 85 100 mole %, and cured at 90 95 oC produced materials with higher strength and elongation at break. SPUU nanocomposites were prepared by maintaining the overall diamine stoichiometry at 95 mole %, and cured at 90 oC. Uniaxial tensile strength was optimized at a particle weight fraction of 1 wt. %, with a nearly 200 % increase in tensile strength and a 40 % increase in elongation at break, compared to pristine SPUU.