This paper investigates the possibility of employing specific protein-polyphenol interactions for encapsulation of polyphenols and flavan-3-ols from green tea extract. Alginate was used for the formation of the particles, along with several types of proteins (whey protein, bovine serum albumin, calcium caseinate, hemp proteins, soy proteins), while ionic gelling was applied as the encapsulation technique, with additional pectin or chitosan coating, in order to reduce the porosity and achieve sustained release of encapsulated ingredients. The formulated particles containing alginate and bovine serum albumin (BSA) or whey proteins exhibited the largest proportion of retained proteins (up to 95% of the initial content), while the combination of alginate with calcium caseinate or whey proteins was the most effective for encapsulation of polyphenols and flavan-3-ols, since that combination of materials enabled to retain the largest content of these compounds in the formulated particles (80%). During the formation of particles no diffusion of polyphenols and flavan-3-ol in the surrounding medium occured, due to the isotonic conditions held during encapsulation, however, significant diffusion and release of proteins from the hydrogel matrix particles occured, resulting in lower protein content retained in the formulated particles. The results suggest that alginate in combination with bovine serum albumin and pectin coating is the most effective for encapsulation of green tea polyphenols and proteins within the particles, which is useful in achieving controlled release of these functional components.