Functional triblock copolymer [polystyrene-b-poly(ethylene-ran-butylene)-b-polystyrene] or SEBS elastomer was used to synthesize flexible organic-inorganic hybrid materials. Modification of elastomer was first achieved via nitration to produce nitrofunctionalized copolymer and its subsequent reduction forming aminofunctionalized copolymer. IR, H-1 NMR and C-13 NMR spectroscopic analyses provided an evidence of their modified structures. Modified SEBS based hybrid materials were then prepared through solution intercalation technique using layered silicates and in-situ polymerization of metal alkoxides via sol-gel process. In the first attempt, hybrids were prepared by the reinforcement of aminofunctionalized SEBS with organophilic montmorillonite to establish compatibility between organic matrix and inorganic phase. Reinforcement of the modified copolymer was secondly achieved by hydrolytic condensation of tetraethoxysilane using 3-glycidyloxypropyl trimethoxysilane (as a coupling agent) yielding hybrid materials. The chemical interactions between the organic polymer chains and the inorganic networks produced in-situ led to better properties of modified elastomer. Mechanical properties of thin transparent films of these hybrids were measured. Tensile strength of hybrids shows a considerable improvement over pure SEBS as well as aminofunctionalized copolymer in all the systems, which shows an increased interfacial interaction between organic and inorganic phases.