Polysaccharide-based soft colloidal particles mediated by the dynamic bonding-engineered interfacial self-assembly can regulate the properties of oil-water interfacial films, availing the stability of emulsions under a wide pH range. The amphiphilic phenylboronic alginate soft colloidal particles (Alg-PBA) were designed to stabilize pH-responsive Pickering emulsions (PEs). Combining stability analysis with quartz crystal microbalance and dissipation monitoring (QCM-D), the microstructure and viscoelasticity of Alg-PBA at the oil-water interface were determined. The results showed that PEs stabilized by Alg-PBA due to a thicker and stronger viscoelastic interface film induced by BO bonds and hydrogen bonds. The structure-function relationship of the Alg-PBA emulsifier driven by dynamic bonds was further elaborated at multiple scales by laser scanning microscopy (CLSM) and scanning electron microscopy (SEM). Meanwhile, the microstructure of aerogels templated by emulsion could be tuned by adjusting dynamic bonds, which provides a new idea for polysaccharide soft material engineering.