Fluorine‐free liquid‐repellent coatings have been highly demanded for a variety of applications. However, rapid formation of coatings possessing outstanding oil repellency and strong bonding ability as well as good mechanical strength (e.g., bendability, impact resistance, and scratch resistance) remains a grand challenge. Herein, a robust strategy to rapidly create fluorine‐free oil‐repellent coatings in only 30 s via rational design of a semi‐interpenetrating polymer network structure is reported. The resulting coating manifests strong bonding capability both in air and underwater. More importantly, it not only provides unprecedented oil repellency, even to high‐viscosity crude oil, but also achieves both excellent bendability and hardness. This simple yet effective design strategy opens up a new avenue to manufacture multifunctional materials and devices with desirable features and structural complexities for applications in sustainable antifouling, drag reduction, nondestructive transportation, liquid collection, and biomedicine, among other areas.

Conductive hydrogels have recently attracted extensive attention in the field of smart wearable electronics. Despite the current versatility of conductive hydrogels, the balance between mechanical properties (tensile properties, strength, and toughness) and electrical properties (electrical conductivity, sensitivity, and stability) still faces great challenges. Herein, a simplified method for constructing hydrophobic association hydrogels with excellent mechanical and electrical properties is proposed. The prepared conductive hydrogels exhibit high tensile properties (≈1224%), high linearity in the whole‐strain–range (R2 = 0.999), and a wide strain sensing range (2700%). The conductive hydrogel can realize more than 1000 cycles of sensing under 500% tensile strain. As an application demonstration, an underwater communication device is assembled in combination with polydimethylsiloxane/Triton X‐100 film coating, which successfully transmits underwater signals and provides warning of potential hazards. This study provides a new research method for developing underwater equipment with excellent mechanical properties and sensing properties.

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