There is currently a renewed interest for improving household and personal-care formulations to provide more environment-friendly products. Fabric conditioners used as softeners have to fulfill a number of stability and biodegradability requirements. They should also display significant adsorption on cotton under the conditions of use. The quantification of surfactant adsorption remains however difficult because the fabric-woven structure is complex and deposited amounts are generally small. Here, we propose a method to evaluate cellulose-surfactant interactions with increased detection sensitivity. The method is based on the use of cellulose nanocrystals (CNCs) in lieu of micron-sized fibers or yarns, combined with different techniques, including light scattering, optical and electron microscopy, and electrophoretic mobility. CNCs are rod-shaped nanoparticles in the form of 200 nm laths that are negatively charged and can be dispersed in bulk solutions. In this work, we use a double-tailed cationic surfactant present in fabric softener. Results show that the surfactants self-assemble into unilamellar, multivesicular, and multilamellar vesicles, and the interaction with CNCs is driven by electrostatics. Mutual interactions are strong and lead to the formation of large-scale aggregates, where the vesicles remain intact at the cellulose surface. The technique developed here could be exploited to rapidly assess the fabric conditioner efficiency obtained by varying the nature and content of their chemical additives.