The present study proposes a novel application of humic substance–aminosilsesquioxane polyelectrolyte complexes (HS–ASQ) as dust suppressants. These complexes are synthesized through the reaction between humic substances (HS) and 3-aminopropyltriethoxysilane (APTES) in aqueous solution, resulting in the formation of active silanol groups that can bind to mineral surfaces and condense, forming gels. The HS–ASQ compositions were found to have a high sorption capacity for dust particles and could form coatings on their surface without cementing the dust, making them potentially useful for environmental applications. The viscosity of the HS–ASQ compositions can be controlled by adding carboxymethylcellulose (CMC), which also enhances their dust suppression abilities. Different compositions of HS–ASQ were synthesized by varying the proportions of APTES and CMC, and dust treated with these samples was assessed for its resistance to wind erosion using a laboratory-scale setup. Treatment with the HS–ASQ composition resulted in substantial reductions in PM10 and PM2.5 concentrations (particulate matter with aerodynamic diameters of 10 µm and 2.5 µm, respectively) of up to 77% and 85%, respectively, compared to the control.