This article reviews the physicochemical aspects of surface-initiated polymer films used to modify planar and non-planar surfaces and to produce micro- and nanoscale patterned features. Particular emphasis is placed on the molecular composition of the polymer and its effect on surface and bulk properties of ultrathin films. Recent advances in the use of responsive polymer films that exhibit dramatically altered properties upon changes in solvent, temperature, or ionic strength are reviewed. The uses of surface-initiated polymer films to modify materials' properties and impact applications in chromatography, nanoparticle-templated synthesis, and carbon nanotube dispersion are highlighted.
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