Pseudobilayer Vesicle Formation via Layer‐by‐Layer Assembly of Hydrophobically Modified Polymers on Sacrificial Substrates

A bilayer of a hydrophobically modified polyelectrolyte, octadecyl poly(acrylamide) (PAAm), sandwiched between the layers of a hydrophilic polyelectrolyte, poly(ethyleneimine) (PEI), is prepared by the sequential electrostatic–hydrophobic–electrostatic‐interaction‐driven self‐assembly on planar and colloid substrates. This process results in a PEI/[PAAm]₂/PEI‐multilayer‐coated substrate. The removal of a PAA/PEI/[PAAm]₂/PEI‐multilayer‐coated decomposable colloidal template produces hollow capsules. Irregular hydrophobic domains of the [PAAm]₂ bilayer in the PEI/[PAAm]₂/PEI‐multilayer capsule are infiltrated with a lipid to obtain a uniform, distinct hydrophobic layer, imparting the capsule with a pseudobilayer vesicle structure.