A novel kind of bottlebrush cellulose-graft-diblock copolymer thermoplastic elastomer (Cell-g-PBA-b-PMMA) was synthesized by grafting from cellulose backbones via surface-initiated atom transfer radical polymerization (ATRP). The mechanical properties of the bottlebrush copolymer elastomers can be adjusted by controlling the block lengths and composition of the side chains.