Elasticity and photoelasticity relationships for polyethylene terephthalate fiber networks by molecular simulationHybrid organic-inorganic materials are of increasing interest in the development of novel materials that unite characteristic properties of both organic and inorganic constituents. This work provides a mechanistic understanding of the processing space necessary to utilize hybrid modifications to produce advanced high strength fibrous and textile materials. The infiltration of organometallic precursors into fiber forming polymers and the subsequent formation of a hybrid material interface is detailed. To explore this in more detail, in-situ quartz crystal microgravimetry is employed to investigate the infiltration of trimethyl aluminum (TMA) into polyethylene terephthalate polymer films. Specifically, films with varied crystallinities are explored demonstrating that an increase in crystallinity results in a decrease in mass uptake of trimethyl aluminum. Subsequently, the authors highlight the structure-property relationships between modified and unmodified fibers infiltrated with TMA. For the first time, increases in peak load and elongation is observed by facile exposure to organometallic vapors. The combined peak load and elongation increase is an exciting outcome typically not observed in synthetic fibers.