Arrancar arcEdit
Ulquiorra is first seen alongside Yammy Llargo when they arrive in Karakura Town to gain information on Ichigo Kurosaki.[6] Yammy comments on his lack of enthusiasm being in the human world, which prompts Ulquiorra to mention that he insisted on coming with him so he shouldn't complain. Yammy apologizes and becomes uneasy that people are starting to gather at the sight they arrived, feeling that they are staring at him. Yammy states he will eat now and uses his Gonzui ability, only to find, much to his displeasure, that the souls are foul tasting. Ulquiorra asks him why he expected such weak souls to taste good and explains to his fellow Arrancar that the humans can't see them, so therefore they couldn't have been staring at him. Yammy admits that he knew before asking who they came to kill. Ulquiorra mentions that they have only come to kill one being and the others can be left alone. When Yammy admits that such a task would be hard. Ulquiorra details that there are currently only three beings of note with any spiritual strength. Upon the arrival of Chad and Orihime Inoue an altercation ensues, resulting in Chad becoming fatally injured.[7] Ulquiorra watches as Yammy attempts to dispatch Orihime, only to be stopped by her Santen Kesshun technique. Then, Yammy notices her Sōten Kisshun technique being used on Chad and questions if she is healing him. Upon noticing this himself Ulquiorra realizes that it is not healing, as it looks more like time reversal or spatial renewal but nothing as simple as healing, making note that he has never seen such a technique before. He then mentions that Orihime is quite strange for a human. When she tries to attack using her Koten Zanshun technique Yammy easily stops it, much to her dismay. Yammy then asks what should be done with her, with Ulquiorra telling him to simply kill her, but he is quickly stopped by the timely arrival of Ichigo.[8]Somewhat confused, Yammy asks Ulquiorra if this is the target they were meant to find. Ulquiorra confirms that he is and applauds Yammy's lack of subtlety as the reason Ichigo became aware of their presence so fast. He then witnesses with feigned surprise as Ichigo effortlessly blocks Yammy's attack and then cuts off the Arrancar's left arm. As Ulquiorra watches the fight between Ichigo and Yammy, he makes note to himself about Yammy's lack of refinement in battle, as he constantly recklessly charges into battle against Ulquiorra's instruction to learn to read his opponents. Though he readily admits that he is surprised that Ichigo was able to cut through Yammy's Hierro and though he has heard that Ichigo has only just recently attained Bankai, he is taken aback that his reiatsu is so solid. However, he reasons to himself that at his current level Ichigo is no threat to Aizen. After Ichigo soundly beats Yammy, Ulquiorra comments that he is struggling and asks if he wants to switch. Yammy tells him to shut up and proceeds to take out his Zanpakutō, causing Ulquiorra to question whether it is actually necessary to use it against Ichigo. [9]
Ulquiorra watches as Yammy attacks a distracted Ichigo until he is saved by the arrival of Kisuke Urahara and Yoruichi Shihōin. After Yammy is effortlessly beaten by Yoruichi and begins to battle Urahara, who fires a blast at Yammy, Ulquiorra steps in and deflects the blast away from them. He then impales Yammy in the stomach with his hand, scolding him for being so reckless and questioning if he knew just who the two he faced are. He mentions that at Yammy's current level he will not win no matter how much he tries. Ulquiorra then opens a Garganta and tells Yammy that it is time for them to retreat. When Yoruichi questions if they are running away, Ulquiorra plainly tells her that she is foolish to make such a taunt, making note that, if the two of them tried to fight him while protecting the others, it is obvious who would emerge the winner. Ulquiorra then states that his mission is over and that he will report to Aizen that the 'fake' Shinigami he was interested in is nothing more than a piece of trash.[10]
Shortly after leaving, Ulquiorra and Yammy arrive back in Hueco Mundo and are greeted by Sōsuke Aizen and an assembly of Arrancar in order to share their findings from the mission to the Human world.[11] Ulquiorra removes his left eye and crushes it, causing it to turn into dust and asks that they all look carefully as it swirls around them, showing them an account of what took place on his mission from his point of view. As Aizen sees for himself, he begins to understand why Ulquiorra chose not to kill Ichigo. As Ulquiorra begins to explain his reasoning, he is interrupted by Grimmjow Jaegerjaquez, who questions his choice to allow Ichigo and his friends live as, regardless of their threat level, they are their enemies. Grimmjow begins to taunt Yammy, but Ulquiorra steps in and ends the building altercation. He then explains that the problem is not Ichigo, as what Aizen is observing is not Ichigo in his current state but his growth rate. Although it is true that his growth rate is quite high, it is disproportionately unstable because it is so immense. He then states that, if they were to just leave him alone, he would eventually destroy himself or become one of their pawns. Grimmjow finds the argument pointless as Ulquiorra could be wrong and he might get powerful enough to get in their way, but Ulquiorra brushes it aside, stating that, if it came to that, he would finish him off himself. Despite the argument, Aizen congratulates Ulquiorra on his work in completing the mission.[12]
A month later Ulquiorra arrives just as Yammy's arm is being reattached. He comments that it was a good idea to bring Yammy's severed arm back though the other Arrancar complains that it will rot as it will take far too long to heal. Yammy then states that it would be nice if their bodies healed on their own like Ulquiorra's eyeballs do. Ulquiorra comments that he should just be happy they could reattach it, as, if his arm was completely destroyed like Grimmjow's was, he would have been kicked out of the Espada as well. Yammy agrees and, after his arm is fixed, they depart as Ulquiorra tells him that Aizen has summoned them.[13] They show up just in time to join several other Espada (including Grimmjow's replacement Luppi Antenor) at the creation of an Arrancar. Ulquiorra asks Aizen what the status of the Hōgyoku is, to which Aizen comments that it is on schedule as far as Soul Society is concerned. He then explains how he is capable of using it at full power, resulting in the creation of Wonderweiss Margela. Aizen then asks Ulquiorra if he remembers the directive he gave him last month. The latter acknowledges that he does, with Aizen placing his full confidence in him to do what he deems necessary to carry out the mission, including allowing him to take whomever he chooses though he insists Grimmjow go along as well.[14]
Ulquiorra then sends Yammy, Wonderweiss, Luppi and Grimmjow to Karakura Town to act as a distraction to the Shinigami while he goes to capture Orihime. As she travels through the waste dimension from Soul Society to the Human world, she is accompanied by two Shinigami. She is startled at the arrival of Ulquiorra via Garganta, who questions Soul Society's use of only two escorts.[15] Though he states that only two guards aren't to his liking, he notes that the disabling of the Koryu is rather convenient for him, as he claims it is not his style to rush a conversation. Before anyone can react, he fatally injures one of the escorts with a Bala blast, which prompts Orihime to use her Sōten Kisshun technique to heal him. Before the other escort can get away, however, he is fatally injured as well by another Bala blast. Orihime widens her field of healing to encompass both injured men. Ulquiorra is amazed at the level of her power and tells her to come with him and not to speak as her answer will have to be yes, for if she says anything else he will kill her. However, he spares her as he reasons that he will kill her friends anyway. He then shows her friends engaged in their own fights elsewhere. Ulquiorra continues explaining that she is not to speak or ask questions as she has no rights; they are not negotiating and it is entirely up to her if her friends die. He then explains that Aizen desires her power and he is under orders to bring her back unharmed.[16]
Ulquiorra arrives just in time in the battle between Ichigo Kurosaki and Grimmjow Jaegerjaquez to stop Grimmjow from releasing his Zanpakutō. He then states that their mission is accomplished and multiple Garganta open up to take back the Arrancar present via Negacion. As they leave, Ulquiorra notices that within Ichigo's reiatsu there are traces of a new power that he has acquired, but is unsure as to what extent.[17]
By threatening her friends' lives, he convinces Orihime to come peacefully, allowing her to say goodbye to one person beforehand. This makes it appear as if she betrayed her friends of her own free will.[18]
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