With the development of nanotechnology, functional amyloid materials draw increasingly attention and plenty of remarkable applications burst out. Amyloids, defining a class of supramolecular assembly of misfolded proteins or peptides into β-sheet fibrils, have evolved many new respects and offered fruitful chemical/biological functions. Such proteinaceous micro/nano-structure provides excellent biocompatibility, rich phase behaviours, strong mechanical properties and stability at an interface not only in nature but also in functional materials, displaying versatile interactions with surfaces/interfaces that have been widely adopted in bioadhesion, synthetic biology and composites. Overall functional amyloids at surface/interface have great capacity for next-generation biotechnology and biomaterials.