The influence of electrostatically-induced heteroaggregation of oppositely charged lipid droplets on the rheology and stability of emulsions has been studied. 20 wt.% oil-in-water emulsions (pH 6) containing oppositely charged droplets were fabricated by mixing cationic lactoferrin-coated lipid droplets with anionic beta-lactoglobulin-coated lipid droplets. Emulsions containing mixtures of droplets with different charges (positive or negative) and sizes (large or small) were prepared, and then their overall particle characteristics (zeta-potential and size) and rheology were measured. Emulsions formed by mixing positive droplets and negative droplets that were both relatively small (d(43) approximate to 0.3 mu m) exhibited extensive flocculation and had paste-like properties at intermediate positive-to-negative particle ratios. On the other hand, emulsions formed by mixing positive droplets and negative droplets that were both relatively large (d(43) approximate to 3 mu m) exhibited little aggregation and had relatively low viscosities at all particle ratios. Emulsions with small negative droplets and large positive droplets (or vice versa), exhibited some aggregation and viscosity enhancement at intermediate particle ratios. The presence of relatively high levels of protein in the aqueous phase of mixed emulsions reduced the level of droplet aggregation and viscosity enhancement observed, which was attributed to the ability of protein molecules to bind to droplet surfaces and neutralize their charges. Electrostatically-induced heteroaggregation of lipid droplets may be a useful means of controlling the physicochemical properties of emulsion-based products in the food, personal care, pharmaceutical and cosmetic industries. (C) 2012 Elsevier Inc. All rights reserved.