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Hypothesis Adsorption of polyelectrolyte brush-grafted nanoparticles (BGNPs) produces a heterogeneous interface with sub-monolayer surface coverage resulting from lateral electrostatic repulsions that limit packing. As a result, the interaction forces between opposing BGNP layers include an adhesive cross-surface BGNP-substrate bridging force that depends on the interparticle spacing, particle size, and strength of electrostatic interactions. We hypothesize that BGNPs with pH-responsive, annealed polyelectrolyte brushes can undergo controlled changes in surface area coverage through post-adsorption swelling or de-swelling into non-equilibrium layer conformations and that such changes in surface coverage can switch off or switch on particle intercalation, bridging attractions, and enhanced energy dissipation upon sliding. This work aims to characterize the nature of surface forces in heterogeneous BGNP adsorbed layers and to utilize pH-sensitive bridging forces as a mechanism to tune friction and adhesion. Experiments Colloidal probe atomic force microscopy (CP-AFM) is used to measure normal and lateral forces between negatively charged silica surfaces with adsorbed pH-responsive cationic BGNPs. The BGNPs are poly(2-dimethylaminoethyl methacrylate) brush-grafted silica nanoparticles. Adhesion force and friction analysis is complemented by simultaneous quartz-crystal microbalance and ellipsometry measurements under conditions that render the particles strongly charged and swollen (acidic) or weakly charged and de-swollen (basic). Findings Adsorbed BGNPs can be swollen or de-swollen via pH rinses, enabling direct control of surface coverage and bridging interactions. Transitions from adhesive bridging contacts with high friction to non-adhesive contacts with low friction forces occur when adsorbed BGNP layers are switched from a de-swollen/weakly charged state to a swollen/highly charged state. The ability to controllably shift the character of normal and lateral forces via coverage-mediated bridging interactions is a unique feature of adsorbed nanoparticulate brush constructs and highlights their potential to condition surfaces with additional functionality compared to dense, planar homopolymer brushes. [ABSTRACT FROM AUTHOR]