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Abstract Despite recent advances in polyelectrolyte systems, designing responsive hydrogel interfaces to meet application requirements still proves challenging. Here, semicrystalline colloidal gels composed of poly(methacrylamide‐co‐methacrylic acid) are investigated in water with storage moduli in the MPa range. A combination of SEM, X‐ray scattering, and NMR reveals the evolution of the colloidal microstructure, crystallinity, and hydrogen bonding with varying monomer ratio. The gels with the finest colloidal microstructure exhibit the most dissipative rheological behavior and are selected for the study of their interfacial characteristics and underlying interactions. Microstructure stabilization and dynamics results from short‐range (attractive) hydrogen bonding and hydrophobic forces, and long‐range (repulsive) electrostatic interactions—the “SALR” pair potential. Further, the gel's surface exhibits a submicron colloidal topography that greatly determines (colloidal‐like) friction as a result of the viscoelastic deformation of the colloidal network, while electrostatic near‐surface interactions propagate in lamellar adhesion. The dynamic and reversible nature of the involved interactions introduces a stimulus responsive behavior that enables the electrotunability of adhesion and friction. This study advances the knowledge necessary to design complex hydrogel interfaces that enable spatial and dynamic control of surface properties, which is of relevance for applications in biomedical devices, soft tissue design, soft robotics, and other engineered tribosystems.