Madame Hydra is Baron Strucker's (new Hydra leader) second in command and the leader of the HYDRA sub-group The Serpent Seven. The role has been filled by many different women including Viper and former SHIELD agent Contessa Valentina Allegro De Fontaine. It could be an interesting to see SHIELD infiltrated by HYDRA having them trying to take the group down by covert methods. The villain had been rumored for The First Avenger but was used in the film's game tie-in instead. Her involvement in Winter Soldier hasn't been confirmed but a cameo could help setup a third film.
Oscar winning actress Jennifer Connelly (A Beautiful Mind) would be my choice to take on the villainess. Her credits include Blood Diamond, Requiem For A Dream, Little Children, Dark City, Labyrinth and Darren Aronofsky's upcoming bible epic Noah. Not to mention the love interest in Joe Johnston's (First Avenger) adventurous Rockeeter. Yes, she played Betty in the original Hulk film but that has no direct connections with the Marvel Cinematic Universe. Ray Stevenson has played both The Punisher and Volstagg, so Connelly playing another Marvel character isn't hard to imagine.
Russian actress Svetlana Khodchenkova (Tinker Tailor Soldier Spy) is portraying Fox's version of the character in The Wolverine who also goes by Viper. However, she won't have ties with either Hydra or Captain America.
Oscar nominated Argentine-French actress Bérénice Bejo (The Artist) is another person I'd love to see in the role.
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