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Novel hybrid, composite polymer electrolytes (HCPEs) based on poly(acrylonitrile‐r‐butadiene) (PAN‐r‐PB), CN‐modified silica nanoparticles (CN‐MSNs), Li triflate, and ionic liquids (ILs) are synthesized. Using a combination of methods, it is demonstrated that these materials segregate into PAN‐rich and PB‐rich phases, the behavior of which changes depending on the IL type. The incorporation of ILs...