A series of living cis-polybutadiene (cis-PB) chains with desired molecular weights could be successfully synthesized during the polymerization process at different monomer conversions or by sequential addition of an extra monomer at every polymerization stage. The amphiphilic silicon hydroxyl-functionalized cis-PB (cis-PB-Si(OH)(3)) could be further achieved via copolymerization of the above living cis-PB chains with ethenyltrimethoxy-silane to obtain trimethoxy silane-functionalized cis-PBs and hydrolysis of these polymers. It is found that the star-shaped cis-PBs were formed by self-assembly via hydrogen bonding interaction from the end-functional groups of -Si(OH)(3). The surface of cis-PB-Si(OH)(3) films transformed from hydrophobic to hydrophilic after water induction at 50 degrees C when the M-n of cis-PB segments was lower than 9.1 kg.mol(-1). The above hydrophilic cis-PB-Si(OH)(3) films exhibit good self-healing behavior at 25 degrees C owing to a great contribution from -Si(OH)(3) hydrophilic terminals. The amphiphilic cis-PB-Si(OH)(3) and its aggregates would have potential application in recyclable elastomers or self-healing elastic coatings with low-temperature resistance.