The present invention provides methods for treating phytoglycogen-containing materials to generate phytoglycogen compositions with enhanced emulsification attribute. One method comprises contacting a phytoglycogen-containing material with at least one protease. The other method comprises heat treatment of a phytoglycogen-containing material, such as corn kernels. The two methods can be applied independently, or can be applied in combination. Applications of phytoglycogen compositions are also included.