For sulfur-crosslinked natural rubber (N.R), my students used to determine the crosslinking density or the percentage of sulfur incorporated by dividing the number of moles of sulfur used initially on the number of moles of N.R which in turn is found by dividing the mass of N.R on the mass of the CRU "constitutional repeating unit" of N.R which is isoprene , as you know. Note that all sulfur is used up as if it is a limiting reactant.
I must add that the famous Ebonite "which is black -usually- polished hard rubber" is N.R that has been vulcanized by using 30-35% sulfur for preferably one hour or more .
A relatively lesser known but more quantitative method is time-domain double quantum NMR. For NR, you can get Mc, i.e. MW between crosslinks but for SBR, you get a paramter which is directly related. 10.1021/ma4026064 (see the title figure)