With downward pressure on the value of almond hulls (AHs), the major byproduct from the largest tree nut crop globally, the streamlined production of several grades of cellulose nanofibrils (CNFs) toward novel aerogels with concurrent sugar extraction was introduced to synergistically drive these products toward commercial adoption. Hot water extraction produced 50% lignocellulose (LC) with equal water-soluble sugars from AH of a soft-shell variety. Aqueous NaOH and NaClO2/KOH treatments isolated ca. 15% alkali cellulose and 12% cellulose, respectively. Coupled 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO) oxidation and blending yielded 88, 91, and 95% LC micro-/nanofibrils (LCMNFs), alkali cellulose nanofibrils (ACNFs), and cellulose nanofibrils (CNFs) with, respectively, 0.76, 1.02, and 0.84 mmol/g surface carboxyls in a similar 4:1 width-to-thickness aspect ratio and ultrahigh length-to-thickness aspect ratios (800-1900). The LCMNF aerogel was mostly wet-resilient, wet-stable, and dry/wet shape-recoverable, whereas the most charged ACNFs gave the stiffest aerogel [31.6 kPa/(mg/cm3)]
