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This study presents a new strategy for achieving ultralow thermal conductivity in nonporous polymer/organic filler hybrids by suppressing heat capacity through tailored atomic vibrations to enhance thermal insulation. Unlike conventional polymer/inorganic filler hybrids, these hybrids exhibit interfacial thermal resistance one to three orders of magnitude lower. Combined experiments and simulations uncover thermal transport mechanisms. These hybrids demonstrate enhanced flame retardancy. Please see the abstract in the attached PDF.

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