It has been established that hydrogen bonds control both gelation and helix formation completely in the case of agarose and partially in the case of kappa-carrageenan, the major role belonging in the latter case to the interactions of a polysaccharide with metal ions. Na+ and K+ ions form contact ion pairs with sulphate groups of kappa-carrageenan. It is supposed that an increase in the number of contact ion pairs together with association of macromolecules having unordered conformation, a decrease in the second virial coefficient, and a decrease in the refraction index increment (i.e., an increase in the solvation degree of dissolved particles) is a necessary condition for forming the kappa-carrageenan gel network. A sufficient condition of kappa-carrageenan gelation is the intermolecular coordination binding of ions such as K+ ions, promoting gelation. The coil-to-helix transition of the polysaccharide is controlled by shielding the charge of kappa-carrageenan-sulphate groups. Hydrophobic interactions proved to be unessential for gelation of either agarose or kappa-carrageenan.