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This work reports a composite film using (3-Aminopropyl)triethoxysilane-modified boron nitride nanosheets (BNNS) incorporated in the aramid nanofibers (ANF) network via sol–gel method. High-resolution TEM, SEM, XPS, and XRD outcomes confirmed the imitation pearl layered structure—BNNSs as thermal conductive fillers were layer-by-layer overlapped on ANF. The reasonable coordination between interfaces and fillers stimulated the thermal conductivity (35.4 W/(m·k)) of composite film i.e., 338.43% higher than that of ANF. The composite film exhibited good cyclic thermal stability, high tensile strength (65.9 MPa), and high volume resistivity (2.424×1015 Ω∙cm). [Display omitted] • BNNS@APTES/ANF with imitation pearl layered structure was prepared via sol–gel method. • BNNS as thermal conductive fillers were layer-by-layer overlapped on the ANF. • High thermal conductivity of BNNS@APTES/ANF was 35.4 W/(m·k) higher than pure ANF. • BNNS@APTES/ANF exhibited excellent tensile property and high volume resistivity. • The thermal conductivity of BNNS@APTES/ANF did not decay during 8 cooling/heating cycles. This work reports a composite film using (3-Aminopropyl)triethoxysilane-modified boron nitride nanosheets (BNNS) incorporated in the aramid nanofibers (ANF) network via sol–gel method. High-resolution TEM, SEM, XPS, and XRD outcomes confirmed the imitation pearl layered structure—BNNSs as thermal conductive fillers were layer-by-layer overlapped on ANF. The reasonable coordination between interfaces and fillers stimulated the thermal conductivity (35.4 W (m·k)-1) of composite film i.e., 338.43 % higher than that of ANF. The composite film exhibited good cyclic thermal stability, high tensile strength (65.9 MPa), and high volume resistivity (2.424 × 1015 Ω∙cm). [ABSTRACT FROM AUTHOR]