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Alright so now that we're at 100 replies time for a little review, if anyone disagrees with any of the following I'd like to know now because I'm looking to catalog what we have so far into a picture. I'll have to ask for a source on some of these. For what "biggest" means please look at the discussions in this thread, but for this purpose it is the character in her universe who has the largest bust in proportion to the rest of her body. Also, as characters often change appearance depending on the artist or the medium the way they look can be from any point in time whether its on a show, a video game, or even as art on a trading card. The one rule being they have to actually be breasts, nothing hard. No implants.
Oh, and one more small note: Don't be fooled by battle armor. Outfits in general can give false impressions as to the true nature of the flesh pillows within.
Quiet-Metal Gear
Passionlip-Fate series
Tsunade (possibly Samui)-Naruto series
Camilla (Possibly Kagero, Tiki)-Fire Emblem Series
Cathyl (Suu may be able to surpass her in one of her forms)-Monster Musume
Selvaria Bles-Valkyria Chronicles
Rangiku (most of the other women are close)-Bleach
Port Demon (Musahsi and Iowa have also been brought up,although it's being argued whether it can be accurately calculated)-Kantai Collection
Wakasagihime-Touhou
Murasaki (although it is being argued that Shiki may far surpass her)-Senran Kagura
Mune Ōmune-Scorching Ping Pong Girls
Magisa (although apparently Sig is close-Granblue Fantasy
Tifa (very specifically during the 3D cutscenes)-Final Fantasy
Baiken-Guilty Gear
Nine-Blazblue
Lorelei-Pokémon
Ivy-Soulcalibur
Valentine-Skullgirls
Bayonetta-Bayonetta
Noriko Kashiwagi-Shin Megami Tensei Series
Jessica Rabbit-Who Framed Rodger
Yoko-Gurren Lagann
Tina-Dead or Alive
Rachel-Ninja Gaiden
Great Fairy-Legend of Zelda
Graf Zeppelin (although Illustrious may be bigger)-Azur Lane
Risky Boots- Shantae
Boa Hancock-One Piece
Part 2 in next post