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Spider-Woman (Jessica Drew) — Eliza Dushku
Joss Whedon is well-known for writing strong female characters, which makes Jessica Drew an ideal character to introduce — though likely without the Spidey costume. Captain America already introduced Hydra, with whom Spider-Woman has ties before becoming a S.H.I.E.L.D. agent, which would make for a great recurring nemesis for Coulson's team. Who better to play an enemy-turned-ally than Buffy and Dollhouse alum Eliza Dushku?