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All-inorganic nanocrystals (NCs) are of great importance in a range of electronic devices. However, current all-inorganic NCs suffer from limitations in their optical properties, such as low fluorescence efficiencies. Here, we developed a general surface treatment strategy to obtain intensely luminescent all-inorganic NCs (ILANs). The absolute photoluminescence quantum yields (PLQYs) of red-, green- and blue-emitting ILANs in polar solvents are 97%, 80% and 72%, respectively, which are the highest among inorganically functionalized NCs. Further study revealed that the passivated Lewis basic sites of ILANs by metal cations boosts the efficiency of radiative recombination of electron-hole pairs. While the passivation of Lewis basic sites leads to a high PLQY of ILANs, the exposed Lewis acidic sites provide the opportunities for directly optically patterning of functional NCs with high-resolution. Our studies provide a new surface engineering approach to design functional NCs and create a versatile platform for patterning NCs.