Reported here for the first time is the alkaline periodate oxidation of lignocelluloses for the selective isolation of cellulose nanocrystals (CNCs). With the high concentrations as ap otassium salt at pH 10, periodate ions predominantly exist as dimeric orthoperiodate ions (H 2 I 2 O 10 4À ). With reduced oxidizing activity in alkaline solutions,dimeric orthoperiodate ions preferentially oxidized non-ordered cellulose regions.The alkaline surroundings promoted the degradation of these oxidized cellulose chains by b-alkoxy fragmentation and generated CNCs.T he obtained CNCs were uniform in size and generally contained carboxyg roups.F urthermore,t he reaction solution could be reused after regeneration of the periodate with ozone gas.T his method allows direct production of CNCs from diverse sources,inparticular lignocellulosic raw materials including sawdust (European beech and Scots pine), flax, and kenaf,inaddition to microcrystalline cellulose and pulp.Supportinginformation and the ORCID identification number(s) for the author(s) of this article can be found under: https://doi.org/10.