Hypothesis: The rheological behavior and frictional properties (macroscopic level) of systems containing a hydrophobically modified polymer and phospholipids depend on the hydrophobic association that occur between the hydrophobic moiety of the polymer and the phospholipid tails (molecular level). The hydrophobicity of the polymer can thus be used to control its interactions with phospholipids, and manipulate complex gel macroscopic behavior. Experiments: By using systems composed of a crosslinked hydrophobically modified polyacrylic acid (HMPAA) or a crosslinked polyacrylic acid polymer (PAA) and phospholipids, we examine the underlying mechanisms through which the components interact using isothermal titration calorimetry (ITC) and their effect on rheological and tribological characteristics of complex gels. Findings: We find the systems containing HMPAA and phospholipid exhibit gel-like behavior with the elastic modulus increasing substantially upon phospholipid addition due to hydrophobic interactions that result in a more interconnected network formation, as evidenced by ITC measurements. Similar experiments with a crosslinked polyacrylic acid polymer (PAA) show no interactions, lending credence to our hypothesis. In addition, soft tribological behavior shows lower friction coefficients at low entrainment speeds with HMPAA concentration and the addition of phospholipid, while no change in friction coefficient was observed in the case of increasing PAA concentration, indicating HMPAA and phospho-lipids to be interacting with the soft PDMS contacts. (C) 2020 Elsevier Inc. All rights reserved.