Oat husks are low-value lignocellulosic residues of oat processing that carry an environmental impact. Their polymers (cellulose, hemicellulose, and lignin) can be converted into a wide variety of value-added products; however, effcient pretreatment methods are needed that allow their fine separation for further tailored valorization. This study pioneered the use of milling-free and low acid-catalyzed ethanol organosolv for the delignification of oat husks, allowing their conversion into three high-quality streams, namely, glucan-rich, lignin-rich, and hemicellulosic compound-rich streams. Temperature, retention time, and solid-to-liquid ratio were found to impact the delignification of oat husks when using a one-factor-at-a-time strategy. The ideal conditions that were found (210 °C, 90 min, and solid-to-liquid ratio of 1:2) culminated into glucan and lignin fractions containing 74.5% ± 11.4% glucan and 74.9% ± 7.6% lignin, respectively. These high-purity lignin fractions open the possibility for higher value applications by lignin, potentially impacting the feasibility of second generation biorefineries. The glucan fraction showed 90% digestibility after 48 h of hydrolysis with 10 filter paper units of enzyme cocktail per gram of glucan. Considering the absence of size reduction and high solid loading, together with the quality of the obtained streams, organosolv pretreatment could be a potential strategy for the valorization of oat lignocellulosic residues. © 2020 by the authors.