This study aims to contribute to the physical understanding of the behavior of nanoparticles in lipid–nanoparticle composite systems. Therefore, composite films were formed on hydrophilic or hydrophobic surfaces through the sequential adsorption of liposomes and silica nanoparticles. The process was performed using dispersions with different pHs by using optical fixed-angle reflectometry. In the first step, liposomes were deposited on the surface, resulting in a lipid monolayer or bilayer depending on the surface’s properties. The kinetic experiments indicated that the adsorption of liposomes is a diffusion-limited process that depends on the pH and the properties of the substrate. In the second step, negatively charged nanoparticles were adsorbed on the membrane as a result of the electrostatic interactions with the positively charged domains on the membrane. The amounts of liposomes and particles adsorbed depend on the charge density of the particles and net charge density of the membrane: an increase in the pH and hydrophobicity of the surface leads to a decrease in the amounts adsorbed because of the increase in the electrostatic repulsion between particles and lipids. The procedure was supplemented with the formation of two liposomes/nanoparticles bilayers.
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