Enhancement in the elastic response of a bacterial thermoplastic elastomer, poly(beta-hydroxyoctanoic-co-undecylenic acid), containing varying amounts of unsaturation was attempted through sulfur vulcanization. Sol-gel analysis verified that crosslinking had occurred and that crosslinking varied with vulcanizing agent type and concentration. Differential scanning calorimetry showed that crosslinking could eliminate all crystallinity. The elastic response was near ideal with less than a 5% tensile set after 200% elongation. In general, sulfur-vulcanized materials exhibited a decrease in tensile modulus, tensile strength and tear resistance which did not appear to vary with crosslink density. Unlike the case of peroxide crosslinking, material integrity was left intact and mechanical property results are reported. The network structure was elucidated through the determination of the molecular weight between crosslinks.