Nitrile N-oxide reagents capable of reacting with unsaturated bonds of rubber polymers and rubber surfaces under catalyst- and solvent-free conditinos, which we have recently developed, are introduced. The synthetic procedure of surface by nitrile N-oxides, and the modification of rubber by the nitrile N-oxide reagents are exhibited. In addition, novel cross-linker samples for vinyl polymers are also shown along with their excellent property.