Developing routes to produce cellulose nanocrystals (CNCs) from high-lignin wood residues is essential for expanding sustainable nanocellulose feedstocks. In this work, Meranti (Shorea sp.) sawdust was valorized into CNCs by integrating ammonium persulfate (APS) pretreatment with subsequent sulfuric acid hydrolysis. To establish a severity map and define an operating window, APS pretreatment severity was systematically varied by adjusting APS concentration and the sawdust-to-APS (solid-to-liquid) ratio, and its influence on CNC structural properties was evaluated. APS pretreatment partially disrupted and oxidized the lignocellulosic matrix, enabling acid hydrolysis to liberate crystalline cellulose domains. XRD analysis confirmed the preservation of the cellulose I crystalline structure, with a maximum crystallinity index of 72% at 2 M APS and a sawdust-to-APS ratio of 1:30 (w/v), and an average crystallite size of approximately 10 nm estimated using the Scherrer equation. SEM and TEM analyses revealed rod-like CNCs with smooth surfaces and relatively homogeneous dimensions. The optimized samples exhibited CNC lengths of 188.71 ± 5.01 nm and widths of 26.79 ± 1.72 nm. These results demonstrate that Meranti sawdust, a high-lignin wood residue, can be converted into structurally well-defined CNCs using a two-step APS/acid process without prior alkaline pulping or bleaching. This study clarifies the role of APS oxidation in enabling CNC production from feedstocks with lignin contents above 20% and provides a basis for valorizing Meranti sawdust as a renewable precursor for CNCs in advanced material applications.
