Grafting of polymer brush (assembly of polymer chains tethered to the substrate by one end) is emerging as one of the most viable approach to alter the surface of inorganic nanomaterials. Inorganic nanomaterials despite their intrinsic functional superiority, their applications remain restricted due to their incompatibility with organic or biological moieties vis-à-vis agglomeration issues. To overcome such a shortcoming, polymer brush modified surfaces of inorganic nanomaterials have lately proved to be of immense potential. For example, polymer brush-modified inorganic nanomaterials can act as efficient substrates/platforms in biomedical applications, ranging from drug-delivery to protein-array due to their integrated advantages such as amphiphilicity, stimuli responsiveness, enhanced biocompatibility, and so on. In this review, the current state of the art related to polymer brush-modified inorganic nanomaterials focusing, not only, on their synthetic strategies and applications in biomedical field but also the architectural influence of polymer brushes on the responsiveness properties of modified nanomaterials have comprehensively been discussed and its associated future perspective is also presented. This article is categorized under: Diagnostic Tools > In Vivo Nanodiagnostics and Imaging Therapeutic Approaches and Drug Discovery > Emerging Technologies Nanotechnology Approaches to Biology > Nanoscale Systems in Biology.