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If I had to choose, it would probably be the episode 31. The subplot with Jack and Carly was handled so nicely, it started to make me like the JackxCarly pairing, which eventually became my favorite Yu-Gi-Oh! pairing, and cemented Jack as my favorite 5D's character after he got some really nice development through his relationship with Carly.
Episode 31 is definitely on my Top 10 best episodes of 5D's. It made Carly be my favorite female character in all of Yu-Gi-Oh!. It's a real shame that Carly forgot what happened about becoming a Dark Signer. They let Kiryu keep his memories of becoming a Dark Signer somehow. I remember that really bothering me.