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Thermal interface materials (TIMs) with high through-plane thermal conductivity (TC), softness, and electrical insulation are highly desired for modern electronics. However, it is challenging to simultaneously achieve these properties. Boron nitride (BN)-based polymer composites are promising candidates for advanced TIMs owing to the high TC and great electrical insulation of BN. However, previous works perform either low TC (< 8 W m−1 K−1) or high stiffness. The ultimate properties of BN-based TIMs remain largely unclear and unrealized. Here, we fabricate BN film-filled silicone rubber composites by a facile stacking-cutting method, which maintains the high degree of orientation the BN film, so that a record-high though-plane TC of 19.1 W m−1 K−1 and a low compressive modulus of 5.42 MPa are achieved. The low BN content (37 vol%) ensures the softness and resilience of the as-prepared TIMs. This work presents a highly efficient strategy to enhance the performance of BN based TIMs, promoting their large-scale manufacturing and practical applications. • Thermal interface materials based on boron nitride film (BNF) were fabricated by a facile stacking-cutting method. • The composites exhibit a high degree of orientation and densely overlapped structures. • The composites show a record-high though-plane TC of 19.1 W m−1 K−1 at 37 vol% BN content and a low compressive modulus of 5.42 MPa. [ABSTRACT FROM AUTHOR]