Thermoplastic elastomers (TPEs) are ever sought using a simple robust synthetic approach. Widely successful first-generation TPEs rely on microphase-separated ABA triblock copolymers (Architecture I). Recent multigraft copolymers represent the second-generation TPEs in which multiple branched rigid segments are dispersed in a rubbery backbone matrix (Architecture II). This paper reports our discovery of the third-generation TPEs that are based on rigid backbone dispersed in a soft grafted matrix. This Architecture III allows the use of random copolymers as side chains to access a wide spectrum of TPEs that cannot be achieved by architecture designs of the first two generations. In this report, random copolymer-grafted cellulose, cellulose-graft-poly(n-butyl acrylate-co-methyl methacrylate) copolymers with only 0.9-3.4 wt % cellulose prepared by activators regenerated by electron transfer for atom transfer radical polymerization (ARGET ATRP), as novel thermoplastic elastomers are investigated.