The sandwich-structured fluorinated graphene (FGN)/poly(vinylidene fluoride-hexafluoro- propylene) [P(VDF-HFP)] composites with various FGN constituents were fabricated via a layer-by-layer solution casting technique, and their dielectric relaxation phenomenons of the trilayered composites were studied in a systematic way by dielectric relaxation spectroscopy (DRS) at various temperatures (25°C–200 °C) in the range of 20 Hz to 5 M Hz. The variations in dielectric parameters (ε′and ε") with frequency at each studied temperature show that ε′and ε" increase with the rise of temperature and ε" significantly decreases with the addition of FGN. Moreover, the asymmetric shapes of electric modulus spectra (M″) and Cole-Cole plots exhibit the relaxation process of non-Debye, especially in trilayered FGN/P(VDF-HFP) composites. AC conductivity is irrelevant to frequency and temperature under low frequency-high temperature, but frequency sensitive under high frequency region. Furthermore, the two activation energies (Eτ and Eσ) gradually increased with the addition of FGN, showing that the mobility of charge carriers is suppressed, thus they are unable to overcome the relaxing and conducing barrier.