Methods of nanoencapsulation are described herein. Embodiments of the method utilize the coacervation of a cationic polyelectrolyte with an anionic polyelectrolyte to form a novel capsular matrix. In particular, the novel methods may be used to encapsulate a suspension of a hydrophobic material such as a carotenoid. The disclosed methods do not require lengthy pH adjustments nor do they require the use of any toxic crosslinking agents. In one embodiment, a method of encapsulation comprises dispersing a hydrophobic compound in an organic solvent to form a solution. The method also comprises admixing an anionic polyelectrolyte and a cationic polyelectrolyte with the suspension to form a mixture. In addition, the method comprises quiescently cooling the mixture so as to cause self-crosslinking of a capsular matrix encapsulating the hydrophobic particles.