Elastomeric networks were prepared from polydimethylsilmethylene (PDMSM) [Si(CH3)2CH2], a polymer closely related to polydimethylsiloxane (PDMSO) [Si(CH3)2O] and polyisobutylene (PIB) [C(CH3)2CH2]. The birefringence of PDMSM in elongation was found to be qualitatively similar to that of PDMSO, in that there was no evidence for strain‐induced crystallization. However, the values of the optical‐configuration parameter Δa were considerably larger, and both Δa and its temperature coefficient are essentially the same as those of PIB. Swelling the PDMSM networks generally decreased Δa; the largest decreases, obtained as expected with the most nearly symmetrical diluent, were also approximately the same as those observed for PIB. Use of cyclic PDMSO pentamer as diluent in a PDMSM network was found to increase the birefringence, presumably because of orientational effects. Various network‐diluent combinations involving the significantly anisotropic PDMSM and the more nearly isotropic PDMSO should be extremely useful for elucidating the nature of these intermolecular correlations. Results obtained from rotational isomeric state theory considerably underestimate both Δa and its temperature coefficient for PDMSM, as they do for PIB. Although the origin of the discrepancy is not necessarily the same for both polymers, the results on PDMSM suggest that the discrepancy for PIB is not due to the severe steric congestion known to be present in this polymer.