This study aimed to elucidate the pathways through which covalent and non-covalent interactions between deamidated gliadin (DG) and tannic acid (TA) on influence the stability of Pickering emulsions. The interactions induced protein unfolding, as evidenced by increased ultraviolet absorption and a red shift in fluorescence emission. DG-TA composite nanoparticles effectively stabilized high internal phase emulsions, whereas DG nanoparticles alone did not. Covalent DG-TA nanoparticle stabilized Pickering emulsions (C-DGTAE) retained a consistent mean droplet size after 30 d of storage. Lipid hydroperoxide and malondialdehyde levels in C-DGTAE and N-DGTAE were reduced by 59.1 %-69.5 % and 38.9 %-44.4 %, respectively. Furthermore, the retention of β-carotene in the emulsions was significantly enhanced. All emulsions exhibited elastic behavior, characterized by higher G' than G". Notably, N-DGTAE demonstrated the highest apparent viscosity, G' and G", attributed to the connected nanoparticles around the droplets. Confocal laser scanning microscopy revealed that C-DGTAE droplets possessed the thickest layer, corroborated by the highest interfacial nanoparticle content of 76 % and an interfacial thickness of 441 nm. These findings suggest that covalent interactions enhance the interfacial nanoparticle layer, while non-covalent interactions promote nanoparticle networking, providing valuable insights for optimizing the stability of Pickering emulsions.