From a circular economy perspective, one-pot strategies for the isolation of cellulose nanomaterials at a high yield and with multifunctional properties are attractive. Here, the effects of lignin content (bleachedvs unbleached softwood kraft pulp) and sulfuric acid concentration on the properties of crystalline lignocellulose isolates and their films are explored. Hydrolysis at 58 wt % sulfuric acid resulted inboth cellulose nanocrystals (CNCs) and microcrystalline celluloseat a relatively high yield (>55%), whereas hydrolysis at 64 wt% gave CNCs at a lower yield (<20%). CNCs from 58 wt % hydrolysis were more polydisperse and had a higher average aspect ratio (1.5-2x),a lower surface charge (2x), and a higher shear viscosity (100-1000x). Hydrolysis of unbleached pulp additionally yielded spherical nanoparticles(NPs) that were <50 nm in diameter and identified as lignin bynanoscale Fourier transform infrared spectroscopy and IR imaging.Chiral nematic self-organization was observed in films from CNCs isolatedat 64 wt % but not from the more heterogeneous CNC qualities producedat 58 wt %. All films degraded to some extent under simulated sunlight trials, but these effects were less pronounced in lignin-NP-containingfilms, suggesting a protective feature, but the hemicellulose contentand CNC crystallinity may be implicated as well. Finally, heterogeneous CNC compositions obtained at a high yield and with improved resourceefficiency are suggested for specific nanocellulose uses, for instance,as thickeners or reinforcing fillers, representing a step toward thedevelopment of application-tailored CNC grades.