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The new proton-conducting composite electrolyte films (PCCEFs) consisting of polyvinyl alcohol (PVA) with varying ammonium fluoride salt concentrations were created using an expanded liquid casting process. The X-ray diffraction (XRD) study confirms the composite electrolyte films (CEFs) formation. The improvement in AMF02 salt doping compared to the PVA matrix film approach resulted in decreased variation in the crystalline size values, thus explaining how [NH4+] and polymer PVA matrix films interact. The band gaps decrease when the AMF02 salt filler concentration increases due to increased crystallite size. The suggested composites evaluated successful CUT-OFF laser filters and attenuation, as well as limiting laser power systems. For the 11.11 wt% AMF02 doping salt, the highest DC conductivity was 73.205 × 10⁻⁹ (siemens/m) at ambient temperature. Our dielectric results demonstrate that the CEFs are usually suitable for optoelectronic systems. There is a huge need to develop low dielectric permittivity composite electrolyte films (CEFs) for microelectronic devices and the high-frequency region.