Intrinsic self-healing polyborosiloxane (PBS) and its multi-walled carbon nanotube (MWCNT)-reinforced nanocomposites were synthesized from hydroxyl terminated poly(dimethylsiloxane) (PDMS) and boric acid at room temperature. The formation of Si-O-B moiety in PBS was confirmed by Fourier transform infrared spectroscopy. PBS and its MWCNT-reinforced nanocomposites were found possessing water or methanol activated mechanically adaptive behaviors; the compressive modulus decreased substantially when exposed to water or methanol vapor and recovered their high value after the stimulus was removed. The compressive modulus was reduced by 76%, 86%, 90% and 83% for neat PBS and its nanocomposites containing 3.0 wt.%, 6.2 wt.% and 13.3 wt.% MWCN...