The combination of ultrasmall nanoparticles and pseudo-single atoms of gold (Au) and fibrous nanosilica (KCC-1) functionalized with 3-aminopropyltriethoxysilane (APTS) enabled the design of KCC-1-APTS/Au nanocatalysts with very high turnover numbers (TONs). KCC-1-APTS/Au catalysed the oxidation of organosilanes to silanols, with a TON of approximately half a million (591 000 for dimethylphenyl silane as a model substrate). Additionally, the figure-of-merit (FOM), which provides an integrated view of the rate of the reaction, the energy required, the reaction scale and the recyclability of the catalysts, was 633 mmol h−1 K−1. KCC-1-APTS/Au also catalysed two additional challenging reactions, the alcoholysis of silane and the hydrosilylation of aldehydes, with very high TONs. These characteristics make KCC-1-APTS/Au a versatile nanocatalyst.