Non-renewable chemical reagents are commonly used as dispersants or flocculants of phyllosilicate clay particles in several industrial fields such as water/wastewater treatment, food production, papermaking, and mineral processing. However, environmentally benign reagents are highly desired due to the non-biodegradability and negative impacts of synthetic reagents on aquatic life. In this work, the dispersion and flocculation behavior of sustainable polymers (anionic and cationic biopolymers) sourced from proteins and polysaccharides were studied in serpentine phyllosilicate suspensions using the following bench-scale tests: zeta potential, microflotation, settling and turbidity, and isotherm adsorption using total organic carbon. The anionic polysaccharide-based biopolymer pectin acted as a switchable biopolymer for serpentine. That is, it could switch from being an efficient flocculant at pH 7 to an effective dispersant at pH 10.