Recent progress in surface-initiated polymerization enables the deliberate polymer modification of nanoscopic surfaces with high levels of precision. This has given rise to the development of brush particle-based materials (sometimes referred to as ‘hairy nanoparticles’) that are formed by tethering of polymer chains to the surface of nanoparticle-like objects. Brush particles have attracted interest as model systems to understand the effect of surface modification on the structure and interactions in polymer modified colloidal systems (which play a role across fields as diverse as functional coatings, cosmetics, foods or pharmaceuticals) but also as building blocks for the assembly of ‘one-component hybrid materials’ that exhibit unprecedented property combinations, not realizable in classical composite materials. This review presents a summary and analysis of the developments in ‘particle brush materials’. The evolution of synthetic methodologies from the original pioneering work to emerging trends and opportunities in the field of brush synthesis is presented first. Subsequently, the effect of brush architecture on the structure, interaction and assembly of brush particles both with and without a matrix is discussed. Finally, recent advances in the development of functional hybrid materials with applications in energy, catalysis, sensing and other areas is presented.