Friction and wear of vast numbers of motion components subjected to varying unlubricated and oil-starved conditions are critical challenges to be addressed. In this work, innovative phenol-formaldehyde resin (PF) composites were formulated by incorporating halloysite nanotubes (HNTs), and their sliding behavior against bearing steel counterparts was systematically investigated using a pin-on-disc tribometer. When sliding takes place under both unlubricated and oil-starved conditions, the PF-based nanocomposites exhibit ultra-low friction and wear. This behavior originates from the formation of multi-layered tribofilms facilitated by synergistic tribo-physical and chemical actions at the sliding interface. Both the Si-Al-based top layer growing at unlubricated interface and the carbon-based top layer growing at oil-starved interface exhibits remarkable solid lubricating performance. This work presents novel design strategies for advanced tribo-composites with varying tribological conditions.