Self-patterning hybrid membranes enable domain-specific immobilization of responsive nanoassemblies.

Biological surfaces often rely on lateral chemical heterogeneity to localize activity and regulate transport, whereas most synthetic polymer membranes remain compositionally uniform. Here, we create active soft surfaces by combining self-patterning hybrid triblock copolymer membranes with stimuli-responsive peptide-based multicompartment micelles (MCMs). The hybrid membranes spontaneously segregate into micron-scale domains with distinct topography, mechanics, and surface chemistry, enabling selective covalent immobilization of MCMs within chemically complementary regions. Cargo loading does not alter the internal architecture of the MCMs, which remains intact upon domain-specific attachment. When heated to 37 °C, the immobilized MCMs undergo thermally induced disassembly, releasing their encapsulated cargo while remaining spatially confined within the membrane domains, thereby inducing temperature-triggered functionality of the surface. This approach establishes a versatile route to engineering programmable surfaces with spatially resolved, stimuli-responsive behavior, providing a platform for controlled release, biosensing, and adaptive interface technologies.