The fascinating tribological phenomenon of carbon nanotubes (CNTs) observed at the nanoscale was confirmed in our numerous macroscale experiments. We designed and employed CNT-containing nanolubricants strictly for polymer lubrication. In this paper, we present the experiment characterising how the CNT structure determines its lubricity on various types of polymers. There is a complex correlation between the microscopic and spectral properties of CNTs and the tribological parameters of the resulting lubricants. This confirms indirectly that the nature of the tribological mechanisms driven by the variety of CNT–polymer interactions might be far more complex than ever described before. We propose plasmonic interactions as an extension for existing models describing the tribological roles of nanomaterials. In the absence of quantitative microscopic calculations of tribological parameters, phenomenological strategies must be employed. One of the most powerful emerging numerical methods is machine learning (ML). Here, we propose to use this technique, in combination with molecular and supramolecular recognition, to understand the morphology and macro-assembly processing strategies for the targeted design of superlubricants.