in my opinion either use them on someone you can max out so that you can get 5* max sig crystals sometimes or pump them into someone that you use alot or pump them into someone who benefits from most from high sig level like Omega Red, Star Lord, Aegon, AA.
You said you have Voodoo. He gets some nice benefits from a higher sig including longer regen, power burn buff on even combos and longer poison and power drain debuffs on odd combos.
For me the top two would be thing-to improve his shielding efficiency or (slightly controversial) AA to get him to the 33% reduction level but if u already have him at that level then maybe SL to improve his damage rampup
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