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Abstract Establishing the independent tunability of transport and mechanical properties in polymer gels would significantly contribute to their implementation as transdermal drug delivery media, among other things. The work conducted herein uses facile changes in the formulation of physically crosslinked styrenic ABA/AB block copolymer organogels to alter their mechanical properties independently from the mass transport of an internally‐loaded nanocarrier. Such independent tunability is made possible by altering the relative amounts of ABA triblock and AB diblock copolymers while holding total copolymer concentration fixed. Specifically, three series of gels each with a fixed total copolymer concentration (10, 20, or 30 wt%) comprised of varying triblock copolymer concentration are studied. Small angle x‐ray scattering confirms that, at the nanoscale, only gel network connectivity changes within each series, while mechanical and release experiments show that increasing network connectivity leads to significant growth of gel moduli, but little change in nanocarrier release rate. 

Abstract Organogels possess characteristics that make them promising materials for enhancing our understanding of nanostructure‐diffusion relationships in gels and for use in diffusion‐centered applications including drug delivery and nanoreactor media. Unlike hydrogels, however, there are no well‐recognized techniques for measuring the fundamental diffusion parameter of diffusivity,D, in organogels. The present work establishes a technique for measuringDbased upon Fourier‐transform infrared spectroscopy. Physically crosslinked gels composed of poly[styrene‐b‐(ethylene‐butylene)‐b‐styrene] and aliphatic mineral oil are used to showcase the new technique's capability. Diffusivity of unimers—oleic acid—and reverse micelles—sodium dioctyl sulfosuccinate (AOT)—within as‐prepared and preswollen gels is quantified and resultant values are commensurate with studies of unimer and micelle diffusion in hydrogels. The case of AOT diffusion is further validated through small‐angle X‐ray scattering analysis, which is in close agreement (<20% difference).