We present a condensed overview of the recent developments of novel responsive thin polymer films from end-tethered chains (polymer brushes), which are different from conventional, uniform, and planar brush layers. For this discussion, we selected two types of recently introduced surface layers: binary brush layers with variable chemical composition forming a controllable gradient of composition and properties in a selected direction and brush layers either grafted directly to inorganic nanoparticles to form hybrid core-shell structures or combined with inorganic nanoparticles embedded into this layer. Unlike traditional brush layers, such a design brings a novel set of responsive surface properties allowing for capillary-driven microfluidic motion, combinatorial-like multiplexing response, reversible aggregation and dis-assembly of nanoparticles, fabrication of ultrahydrophobic coatings, and switchable mass transport across interfaces.