Cellulose nanocrystals (CNCs) are unique, renewable top-down nano particles from which coatings with improved gas barrier properties and new functionalities can be prepared. In this paper, the potential for obtaining such high performing nanocrystals from low-cost lignocellulosic by-products or raw materials is proved by a comparison study on CNCs obtained both from cotton linters and kraft pulp, by means of the ammonium persulfate (APS) process. Morphological and chemical characterization of the nanocrystals obtained, as well as the main functional properties of the poly(ethylene terephthalate) coated films, showed quite similar characteristics and performances of CNCs obtained from pure cellulose raw material (cotton linters) and the nanoparticles produced from a potential discard of paper making processes (kraft pulp). In particular, the gas barrier properties of the coating produced with CNCs obtained from kraft pulp were very promising, providing oxygen and carbon dioxide permeability values hundreds of times lower than those of equal thickness in comparison with common barrier synthetic polymers, over a broad range of temperatures. The results obtained are relevant not only for the outstanding performances achieved, but also because they evoke a possible positive example of industrial symbiosis in the packaging field, merging together the requirements and needs of the paper and plastic industries and addressing the way towards a better management of waste and materials.