There is a growing interest to design biomimetic self-assembled composite films from renewable resources aimed at a combination of high toughness, strength and stiffness. However, the relationship between interfacial interactions of the components and the mechanical performance of the composite is still poorly understood. In this work we present evidence of the link between mechanical performance of carbohydrate-based composites with nanolubrication and with direct surface forces between the hard and soft domain in the system. Our approach was to use nanofibrillated cellulose (NFC) as the major reinforcing domain and to modify it by adsorption of a small amount of soft polyethylene glycol grafted carboxymethyl cellulose (CMC-g-PEG). The effect of the soft polymer on direct normal and friction forces in air between cellulose surfaces was evaluated using colloidal probe microscopy. The fibrillar structure of the NFC thin film affected the frictional behaviour; when decreasing load, the friction between pure cellulose surfaces increased, suggesting partial pull-out of fibrils, a phenomenon not observed for non-fibrillar cellulose substrates. Adsorption of CMC-g-PEG on both surfaces decreased the friction considerably but adhesion was still high. The symmetric system, having both cellulose substrates covered with the polymer, was compared to asymmetric systems where only one surface was covered with the polymer. Furthermore, a free standing composite film was prepared by non-ionic self-assembly of NFC and CMC-g-PEG with 99 : 1 weight-ratio; the mechanical properties of the macroscopic films were related to the nanoscaled interactions between the components. The composition studied showed excellent mechanical properties which do not follow the simple rule of mixture. Thus, a synergy in the direct surface forces and mechanical properties was found. This approach offers a robust path to aid in the efficient design of next generation biomimetic composites.