This article critically reviews the fundamental scientific tools, as well as constructs cohesive schemes for potential applications, relevant to the molecularly-thin liquid film technology. Our focus is to understand the nanoscale dynamic behavior of thin lubricant films, relevant to the emerging field of nanotechnology, especially for achieving durability and reliability in the nanoscale devices. Our goal is to present a unified and hybrid description of perfluoropolyether (PFPE) experiment, mesoscopic interpretation, microscopic simulation tools, and molecular design tools available up to now. The experimentation and theory for the physicochemical properties of ultra-thin PFPE films are used to examine liquid film in the sub-monolayer to multilayer regime. Methods for extracting spreading properties from the scanning microellipsometry (SME) for various PFPE/solid surface pairs and the surface rheological characterization of PFPEs are examined. The interrelationships among SME spreading profiles, rheology, surface energy, and tribology, are given. Mesoscopic theories, including thermodynamics of evaporation and flow, stability analysis, microscale mass transfer, and capillary waves are introduced to describe thin PFPE film dynamics. Estimation of thin film viscosity enhancement from vapor pressure suppression by dispersion force is reviewed. The method for experimental derivation of lubricant spreading profiles from contact angles is summarized. The implications of capillary waves, or thermal fluctuations, at the surface of polymeric lubricant films are also discussed. The lattice-based, simple reactive sphere Monte Carlo (MC) technique for examining the fundamentals of PFPE dynamics is illustrated. An off-lattice based bead-spring MC model is also introduced to capture a detailed internal structure of the PFPE molecules, and the molecular dynamics method is implemented for a full-scale nanostructural analysis of PFPE ultra-thin films. By systematically tuning the endgroup strengths of PFPE, we examined the physicochemical properties for thin liquid films of the various PFPE/solid surface pairings. These tools accurately describe the static and dynamic behavior of ultra-thin liquid films consistent with experimental findings and thus are suitable for examining the fundamental mechanisms of lubrication in nanoscale devices. Application of the next generation head-disk interface design in information storage device is briefly considered.