Modern devices require the tuning of the size, shape and spatial arrangement of nano-objects and their assemblies with nanometre-scale precision, over large-area and sometimes soft substrates. Such stringent requirements are beyond the reach of conventional lithographic techniques or self-assembly approaches. Here, we show nanoscale control over the fluid instabilities of optical thin glass films for the fabrication of self-assembled all-dielectric optical metasurfaces. We show and model the tailoring of the position, shape and size of nano-objects with feature sizes below 100 nm and with interparticle distances down to 10 nm. This approach can generate optical nanostructures over rigid and soft substrates that are more than tens of centimetres in size, with optical performance and resolution on a par with advanced traditional lithography-based processes. To underline the potential of our approach, which reconciles high-performance optical metasurfaces and simple self-assembly fabrication approaches, we demonstrate experimentally and via numerical simulation sharp Fano resonances with a quality factor, Q, as high as similar to 300 in the visible for all-dielectric nanostructures, to realize protein monolayer detection.