It is well known that deuteron nmr is a very sensitive tool for the investigation of order and orientation. H-1 and H-2 nmr measurements of partially deuterated poly(butadiene) elastomers with systematically varied elastic properties are presented. A combined study of proton and deuteron nmr relaxation and the behavior under mechanical deformation was performed. H-2 nmr transverse magnetization data are compared to the predictions of a model describing elastomer deuterium transverse magnetization data as a linear superposition of contributions from elastic chains and free dangling chain ends. The structural parameters are compared with results from mechanical and swelling measurements. The influence of microstructure. precursor chain length and their molar mass distribution as well as of the crosslink density on the transverse relaxation and the deformation behavior were studied. (C) 2000 Elsevier Science Ltd. All rights reserved.