Supramolecular interactions such as hydrogen bonds have seldomly considered to be strong enough to maintain dimensional stability of elastomers. Herein, the interplay between spacer length and oligopeptide binding have been used to harvest a strong and stable polyisoprene elastomer comparable to vulcanized counterpart. It is found that along the increase of spacer length from 3 to 5 and 7, the mechanical strength and thermostabilities of elastomers increased remarkably with the maintenance of high extensibility. The high apparent activation energies and obviously reduced relaxation rate could account for the observed phenomenon. This case indicates that the architecture control of polymer could coordinate with supramolecular interactions and broaden their applications.