This report details how sequential crosslinking processes can be applied to develop properties in sulfur-bisphenol A composites. Olefinic carbons were first crosslinked by inverse vulcanization (InV) at 180 C and then aryl carbon crosslinking was affected via radical-induced aryl halide-sulfur polymerization (RASP) at 220 C. To demonstrate that these two crosslinking mechanisms are orthogonal and can be used to affect stepwise property changes, O,O 0-diallyl-2,2 0 ,5,5 0-tetrabromobisphenol A was selected as a comonomer. After InV of the monomer with 90 wt% sulfur, a flexible plastic material having an elongation at break of 89% was obtained, whereas after heating this premade polymer to initiate RASP, the polymer develops a threefold increase in its tensile strength and has an elongation at break of only 29%. The sequential crosslinking strategy demonstrated herein thus provides an innovative approach to tuning the properties of high sulfur-content materials.