The global textile industry has an ongoing need for improved softening products. Current materials systems, including those with siloxane polymers, exhibit certain limitations such as yellowing, high cost, and low softening efficiency. Investigations into fabric softening mechanisms invoke molecular modeling tools to simulate siloxane polymer and cotton fiber interactions at the molecular level. This research describes how certain polymer types exhibit fundamentally enhanced siloxane and fiber interactions within particular pH ranges. Molecular modeling results are also correlated with empirical findings. The output of this research adds insight into efforts to understand fabric softening phenomena.Siloxanes have low surface energy, excellent lubricity, heat stability, and limited solubility in organics, coupled with water insolubility. At the molecular level, the fabric softening properties of siloxanes are believed to be derived from the flexibility of the siloxane backbone [ 12] that results from the freedom of rotations about the Si--O-Si linkages and the low interaction energies of the methyl groups. At room temperature, there is virtually no energy barrier to prevent molecular flexing [ 12,13]. Consequently, siloxanes act as highly effective lubricants in reducing fiber-on-fiber friction. Siloxane functional groups provide strong attractive interactions between the fabric softener and the cotton surface, without which the softener would wash off over time.To enhance interactions between siloxanes and textile materials to increase durability during processes such as washing, reactive siloxanes and modified, nonfunctional siloxane structures are used [ 19]. Indeed, modifying nonfunctional siloxane structures by replacing pendant or terminal methyl groups with various organic functional groups brings a wide range of physical properties to the siloxane polymers. Amino functional groups play an important role in providing enhanced softening properties to organosilicone compounds [8]. In practice, amino functional silicones are widely used in the textile industry as premium-grade fabric softeners [9, 18, 1].Because of the interactions of amino groups with textile materials, amino functional siloxanes are physically adsorbed onto fiber surfaces. This adsorption feature improves the durability of amino functional siloxane fabric softeners during the washing process. The amino groups become cationic (-NH3+) at acidic conditions, and the ionization provides strong attractions to the fabric. The physical properties of typical aminoalkyl functional siloxanes have been described in detail in the literature [ 17]. The objective of this work is to gain a better understanding of the basic softening phenomena of aminoalkyl functional siloxanes on cotton fabrics. Specifically, this report discusses the effect of pH on softening efficiency derived from aminoalkyl functional siloxanes. Molecular modeling results relate experimental observations with chemical and intermolecular interactions to study the softening mechanism.