Graft copolymerization of several vinyl monomers onto polyisoprene was carried out to explore the possibility to recycle waste rubber to useful functional materials. Synthetic polyisoprene, vulcanized natural rubber, and vulcanized natural rubber with carbon black were converted to lower molecular weight polymers at 300°C, under air or nitrogen atmosphere. The obtained low molecular weight natural rubber and polyisoprene were soluble in organic solvents, such as hexane, toluene, tetrahydrofuran (THF), chloroform, and monochlorobenzene. Radical copolymerization of styrene with a thermally fragmented natural rubber was carried out at 80°C in bulk for 2 h in the presence of 2,2Ј-azobis(isobutyronitrile) (AIBN) under air atmosphere to give the corresponding grafted copolymer. The obtained polymer was a beige powdery copolymer at room temperature and consisted of isoprene (38 mol %) and styrene (62 mol %) units, respectively.