High-performance　multifunctional　polymeric　materials　integrated　with　high　fire　safety,　excellent　mechanical　performances　and　electromagnetic　interference　(EMI)　shielding　properties　have　great　prospects　in　practical　applications.　However,　designing　highly　fire-safe　and　mechanically　robust　EMI　shielding　nanocomposites　remains　a　great　challenge.　Herein,　hierarchical　thermoplastic　polyurethane/cyclophosphazene　functionalized　titanium　carbide/carbon　fiber　fabric　(TPU/CP-Ti3C2Tx/CF)　nanocomposites　with　high　fire　safety　and　mechanical　strength　and　toughness　were　prepared　through　the　methods　of　melt　blending,　layer-by-layer　stacking　and　thermocompression.　The　TPU/CP-Ti3C2Tx　showed　improved　thermal　stability.　Moreover,　the　peak　of　heat　release　rate　and　total　heat　release　of　the　hierarchical　TPU　sample　containing　4.0　wt.%　CP-Ti3C2Tx　were　respectively　reduced　by　64.4%　and　31.8%　relative　to　those　of　pure　TPU,　which　were　far　higher　than　those　of　other　TPU-based　nanocomposites.　The　averaged　EMI　shielding　effectiveness　value　of　the　hierarchical　TPU/CP-Ti3C2Tx-2.0/CF　nanocomposite　reached　30.0　dB,　which　could　satisfy　the　requirement　for　commercial　applications.　Furthermore,　the　tensile　strength　of　TPU/CP-Ti3C2Tx-2.0/CF　achieved　43.2　MPa,　and　the　ductility　and　toughness　increased　by　28.4%　and　84.3%　respectively　compared　to　those　of　TPU/CF.　Interfacial　hydrogen　bonding　in　combination　with　catalytic　carbonization　of　CP-Ti3C2Tx　nanosheets　and　continuous　conductive　network　of　CF　were　responsible　for　the　superior　fire　safety,　excellent　EMI　shielding　and　outstanding　mechanical　performances.　This　work　offers　a　promising　strategy　to　prepare　multifunctional　TPU-based　nanocomposites,　which　have　the　potential　for　large-scale　application　in　the　fields　of　electronics,　electrical　equipment　and　5　G　facilities.　©　2023