In order to improve the surface compatibility of bamboo pulp fibers (BPF) with plastic materials, enlarge the application fields, BPF macromolecule which was modified by 2-bromoisobutyryl bromide (BIBB) was chosen as the initiator. Copper(II)bromide/ N,N,N’,N’,N’-pentamethyldiethylenetriamine (PMDETA) was used as the catalyst and ascorbic acid was selected as the reducing agent. Surface grafting modification of BPF with monomer isoprene was prepared by the method of Activators Regenerated by Electron Transfer Atom Transfer Radical Polymerization (AGET-ATRP), meanwhile the effects of parameters such as monomer content, catalyst content, response time and temperature on modification were determined. The results showed that the significant changes of the surface chemical groups in FTIR spectrogram demonstrated the occurrence of grafting reaction and monomer isoprene was successfully grafted onto the surface of BPF. And the changes in XRD spectrogram showed the changes of crystal structure, which verified the veracity of the results.