Bovine serum albumin (BSA)-epigallocatechin-3-gallate (EGCG) have been widely studied; however, the effects of EGCG concentration on the properties of these complexes and their influence on the stability of high-internal-phase Pickering emulsions (HIPPEs) remain limited. This study aims to reveal the interactions between BSA and varying concentrations of EGCG and the application of BSA-EGCG complexes for creating stable emulsions. As the concentration of EGCG decreases from 0.3% to 0.1%, the β-sheet content significantly increased and the β-turn content significantly decreased, resulting in smaller sizes and zeta potentials of 50 μm and −58.7 mV, respectively, at a 0.1% EGCG concentration. This change enhances the ability of BSA-EGCG to adsorb at the oil-water interface, effectively lowering interfacial tension and increasing the emulsion viscosity. Moreover, the interactions between BSA and EGCG markedly improved pH stability, ionic stability, thermal stability, centrifugal stability, and freeze-thaw stability of emulsions. These findings highlight the valuable role of EGCG levels on BSA-EGCG interactions and formed HIPPEs, suggesting their promising applications in the food and pharmaceutical industries.