Composite　organohydrogels　have　been　widely　used　in　wearable　electronics.　However,　it　remains　a　great　challenge　to　develop　mechanically　robust　and　multifunctional　composite　organohydrogels　with　good　dispersion　of　nanofillers　and　strong　interfacial　interactions.　Here,　multifunctional　nanofiber　composite　reinforced　organohydrogels　(NCROs)　are　prepared.　The　NCRO　with　a　sandwich-like　structure　possesses　excellent　multi-level　interfacial　bonding.　Simultaneously,　the　synergistic　strengthening　and　toughening　mechanism　at　three　different　length　scales　endow　the　NCRO　with　outstanding　mechanical　properties　with　a　tensile　strength　(up　to　7.38　±　0.24 MPa),　fracture　strain　(up　to　941　±　17%),　toughness　(up　to　31.59　±　1.53 MJ m−3)　and　fracture　energy　(up　to　5.41　±　0.63 kJ m−2).　Moreover,　the　NCRO　can　be　used　for　high　performance　electromagnetic　interference　shielding　and　strain　sensing　due　to　its　high　conductivity　and　excellent　environmental　tolerance　such　as　anti-freezing　performance.　Remarkably,　owing　to　the　organohydrogel　stabilized　conductive　network,　the　NCRO　exhibits　superior　long-term　sensing　stability　and　durability　compared　to　the　nanofiber　composite　itself.　This　work　provides　new　ideas　for　the　design　of　high-strength,　tough,　stretchable,　anti-freezing　and　conductive　organohydrogels　with　potential　applications　in　multifunctional　and　wearable　electronics.[Figure　not　available:　see　fulltext.]　©　2023,　The　Author(s).