Aqueous lubrication has emerged as an active research area in recent years due to its prevalence in nature in biotribological contacts and its enormous technological soft-matter applications. In this study, we designed aqueous dispersions of biocompatible whey-protein microgel particles (WPM) (10-80 vol %) cross-linked via disulfide bonding and focused on understanding their rheological, structural and biotribological properties (smooth polydimethylsiloxane (PDMS) contacts, R < 50 nm, ball-on-disk set up). The WPM particles (D = 380 nm) displayed shear-thinning behavior and good lubricating performance in the plateau boundary as well as the mixed lubrication regimes. The WPM particles facilitated lubrication between bare hydrophobic PDMS surfaces (water contact angle 108°), leading to a 10-fold reduction in boundary friction force with increased volume fraction (ϕ ≥ 65%), largely attributed to the close packing-mediated layer of particles between the asperity contacts acting as "true surface-separators", hydrophobic moieties of WPM binding to the nonpolar surfaces, and particles employing a rolling mechanism analogous to "ball bearings", the latter supported by negligible change in size and microstructure of the WPM particles after tribology. An ultralow boundary friction coefficient, μ ≤ 0.03 was achieved using WPM between O plasma-treated hydrophilic PDMS contacts coated with bovine submaxillary mucin (water contact angle 47°), and electron micrographs revealed that the WPM particles spread effectively as a layer of particles even at low ϕ∼ 10%, forming a lubricating load-bearing film that prevented the two surfaces from true adhesive contact. However, above an optimum volume fraction, μ increased in HL+BSM surfaces due to the interpenetration of particles that possibly impeded effective rolling, explaining the slight increase in friction. These effects are reflected in the highly shear thinning nature of the WPM dispersions themselves plus the tendency for the apparent viscosity to fall as dispersions are forced to very high volume fractions. The present work demonstrates a novel approach for providing ultralow friction in soft polymeric surfaces using proteinaceous microgel particles that satisfy both load bearing and kinematic requirements. These findings hold great potential for designing biocompatible particles for aqueous lubrication in numerous soft matter applications.