A convenient and sustainable protocol for the aerobic oxidation of benzyl alcohols to carbonyl compounds, based on the use of 1,2,4-triazole-type ligands and nickel(II) bromide, is described. This combination leads to the formation of an exceedingly active, enzyme-like system that allows for other oxidative processes, such as benzylic C–H oxidation and oxygen-mediated cleavage of C–C triple bond, a pioneering procedure for transformation of alkynes into carboxylic acids.