The 1920s was a decade of great change and upheaval, with monstrous demons appearing across America. To combat this menace, the holy organization known as the Order of Magdalene was established. The organization's New York branch is home to the young and reckless Sister Rosette Christopher, as well as her partner Chrno. Tasked with the extermination of demonic threats, the renowned team is excellent at their job, despite causing extensive collateral damage on their missions. However, both Rosette and Chrno are driven by their dark pasts. Through exterminating demons, Rosette hopes to find her lost brother Joshua who was taken by the sinner and demon, Aion, with whom Chrno also shares a bloody history. The two of them must fight off the increasingly dangerous demonic menace and discover its source, while continuing to search for the truth behind Joshua's disappearance.

Unaired episode 12 included with volume 4 of the BD/DVD release.

When Mizuki Hijiri transferred to a new school, all she wanted was to live a normal school life, but that did not prove to be the case when she met the infamous Hero Club. All of its members are boys suffering from various types of chuunibyou—Yamato Noda is a righteous hero, using his athletic abilities to perform noble deeds and protect others; Kazuhiro Nakamura claims to be the reincarnation of Touga Ryushouin, the result of the forbidden union between a demon and an angel; Tomoki Takashima is a pretty-boy otaku whose one true love is the 2D anime girl Sora; and Rei Tsukumo plays the role of a schemer, covertly pulling the strings. Dragged along as the newest member of the Hero Club, tepid Hijiri can't obtain the normalcy that she desires. But even so, despite their various quirks, their bonds of friendship are real; Hijiri's life can only get more exciting when she joins in on their delusions of grandeur!

The awkward lovebirds, Yuuta Togashi and Rikka Takanashi are now living together as they enter a new school year, but their adorable relationship remains stagnant. Yuuta struggles to adapt to having a chuuni girlfriend while the gang—Sanae Dekomori, Shinka Nibutani and Kumin Tsuyuri—are still keeping up with their quirks despite having advanced a grade. Making matters worse, another chuuni girl from Yuuta's middle school, Satone Shichimiya, appears... With the various events revolving around Yuuta, will he be able to develop his relationship with Rikka?