As noncovalent chalcogen-bonding interaction is comparatively weak, it remains a true challenge to implement chalcogen-bonding catalysis in an efficient manner. We herein show that a chalcogen-bonding catalysis approach to cyanosilylation of a broad range of ketones can be achieved even using as low as parts per million (ppm) level catalyst loading while the reactions were completed within several minutes at room temperature. Considering the nature of weak noncovalent forces, this chalcogen-bonding catalysis approach is remarkable as it can give up to 10 6 /h turnover frequency numbers.