Hydrophobic composites are prepared from Ultra High Molecular Weight Polyethylene (UHMWPE) and onion-like carbon (OLC), employing a solvent-free mechanochemical process consisting of milling at 250 rpm for 60 min. The encapsulation of OLC on the surface of UHMWPE microspheres increased with the increasing composition of OLC from 0.5 to 5 wt.%, thereby mimicking the core-shell structure. The consolidated composite with 5 wt.% of OLC exhibited a higher water contact angle (WCA) of about 111.18°, compared to pure UHMWPE (94.80°).