Various embodiments disclosed related to modified elastomer surfaces and methods of making and using the same. In various embodiments, the present invention provides a method of modifying the surface of an elastomer. The method can include contacting a polymerizable composition and at least part of a surface of an elastomer. The polymerizable composition can include a free-radical polymerizable monomers, an organoborane-organonitrogen free-radical initiator, and an amine-reactive compound. The method can include at least partially polymerizing the polymerizable composition, to provide a polymerization product of the polymerizable composition on the surface of the elastomer.