In the present study, the main objective was to valorise industrial agro-wastes for the obtaining of value-added nanocellulose. To the best of our knowledge, no report on the preparation of CNC from garlic straw residues is available in the literature. Therefore, the main objectives of the present work were characterization of garlic straw, its pretreatment and the extraction and characterization of cellulose nanocrystals in order to test its potential value-added utilization as a new source of cellulosic fiber based materials.