A linear anionic polysaccharide, sodium alginate, electrostatically interacts with a cationic polysaccharide, quaternized hydroxyethyl cellulose ethoxylate, in aqueous solution, thus giving an interpolyelectrolyte complex. Aqueous solutions of the initial polysaccharides and polycomplexes with an excess of the cationic or anionic polymers were used for the stabilization of soil and sand against water erosion. Physicochemical, mechanical and biological properties of the polymers and coatings were characterized by gravimetric analysis, viscosimetry, mechanical strength assessment, cell viability, and cell-mediated degradation with the following main conclusions. (a) Non-stoichiometric polycomplexes with an excess of cationic or anionic units (“cationic” and “anionic” polycomplexes, respectively) form transparent solutions or stable-in-time dispersions. (b) The complexation results in a decrease in the viscosity of polymer solutions. (c) A complete dissociation of polycomplexes to the initial components is achieved in a 0.2 M NaCl solution. (d) Soil/sand treatment with 1 wt% aqueous solutions of polymers or polycomplexes and further drying lead to the formation of strong composite coatings from polymer(s) and soil/sand particles. (e) Cationic polycomplexes form stronger coatings in comparison with anionic polycomplexes. (f) The polymer–soil coatings are stable towards re-watering, while the polymer–sand coatings show a much lower resistance to water. (g) The individual polysaccharides demonstrate a negligible toxicity to Gram-negative and Gram-positive bacteria and yeast. (h) The addition of Bacillus subtilis culture initiates the degradation of the polysaccharides and polycomplexes. (i) Films from polysaccharides and polycomplexes decompose down to small fragments after being in soil for 6 weeks. The results of the work are of importance for constructing water-resistant, low toxicity and biodegradable protective coatings for soil and sand.