Nowadays, there is an increasing consumer demand for more natural and environmentally friendly food additives. The current research aimed to produce and characterize a new additive based on bentonite and the phenolic compounds from green propolis extract, as well as to characterize the effect of this additive on the rheological properties of carrageenan hydrogels. The new additive (biohybrid) was obtained after the adsorption of phenolic compounds on the clay platelets. The adsorption mechanism was explained by Langmuir and Freundlich models, which suggested that adsorbed phenolic compounds form a monolayer and multilayers on the clay surface. Despite phenolic adsorption, the physico-chemical attributes of the bentonite remained unchanged. The incorporation of the biohybrid (BH) increased the sol-gel transition temperature of carrageenan hydrogels. This research reports for the first time the development and application of a new natural ingredient with potential food applications.