This research introduces a sustainable method for extracting carboxymethyl cellulose (CMC) from durian peel waste via supercritical carbon dioxide (Sc.CO2) processing, leading to the development of advanced aerogel scaffolds. The study evaluates the influence of Sc.CO2 treatment times (60, 90, and 120 min) on the properties of the produced CMC, investigating enhancements in terms of thermal stability, crystallinity, and mechanical attributes through thermogravimetric analysis (TGA), differential scanning calorimetry (DSC), and mechanical strength assessments. It was discovered that a 90-minute treatment duration yielded CMC aerogels with notable improvements in porosity, structural robustness, and mechanical resilience. This innovative approach not only proposes a viable strategy for repurposing agricultural by-products but also significantly augments the functional qualities of CMC aerogels, rendering them highly applicable in diverse fields. The outcomes underscore the efficiency of Sc.CO2 treatment in refining the mechanical and thermal characteristics of CMC derived from durian peel waste, facilitating the creation of aerogel scaffolds poised for use in various sectors including drug delivery, water purification, and eco-friendly packaging, thereby contributing to the global initiatives for sustainability and efficient waste management.