Lubrication is the key to efficient function of human tissues and has significant impact on the comfort level. However, the construction of a lubricating nanofibrous membrane has not been reported as yet, especially using a one-step surface modification method. Here, bioinspired by the superlubrication mechanism of articular cartilage, we successfully construct hydration-enhanced lubricating nanofibers via one-step in situ grafting of a copolymer synthesized by dopamine methacrylamide (DMA) and 2-methacryloyloxyethyl phosphorylcholine (MPC) onto electrospun polycaprolactone (PCL) nanofibers. The zwitterionic MPC structure provides the nanofiber surface with hydration lubrication behavior. The coefficient of friction (COF) of the lubricating nanofibrous membrane decreases significantly and is approximately 65% less than that of pure PCL nanofibers, which are easily worn out under friction regardless of hydration. The lubricating nanofibers, however, show favorable wear-resistance performance. Besides, they possess a strong antiadhesion ability of fibroblasts compared with pure PCL nanofibers. The cell density decreases approximately 9-fold, and the cell area decreases approximately 12 times on day 7. Furthermore, the in vivo antitendon adhesion data reveals that the lubricating nanofiber group has a significantly lower adhesion score and a better antitissue adhesion. Altogether, our developed hydration-enhanced lubricating nanofibers show promising applications in the biomedical field such as antiadhesive membranes.