Radio frequency (r.f.) plasma polymerization of vinylidene fluoride (CH2CF2) has been used to modify the surface properties of chlorobutyl rubber. FTIR-ATR spectra of the treated rubbers and transmission spectra of plasma polymer films on NaCl windows indicated that as power increased the F/H ratio decreased. SIMS tests supported the FTIR results, and showed that the decrease in the F/H ratio was due to a decrease in the amount of F and an increase in the amount of H in the plasma polymer. Sliding friction measurements showed a reduction in the coefficient of friction (μ) from 3.7 for the untreated rubber to values ranging between 0.4 and 1.9 for the plasma-treated rubbers. There did not appear to be any correlation between the coefficient of friction and plasma power or monomer flow rate, and the average coefficient of friction for the plasma-treated samples was 0.9, which was lower than a commercially used silicone oil treatment (μ = 1.1–1.3). Repetitive sliding friction tests showed that the plasma- and silicone oil treated-chlorobutyl rubbers had the similar lubricating lifetimes. © 1997 John Wiley & Sons, Inc. J Polym Sci B: Polym Phys 35: 1651–1660, 1997