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Series By Tite Kubo
Ulquiorra is a slender, yet fairly muscular, male Arrancar of average height with a melancholic appearance, fairly short, messy black hair, grayish skin, a black upper lip, and green eyes with slit-shaped pupils. One of his bangs falls between his eyes, somewhat similar to Rukia Kuchiki, and he has distinctively thick eyebrows. He has teal lines that descend from his eyes, making it appear as if he is crying. His facial expression rarely changes, and he is almost always frowning. He wears typical Arrancar clothes: a white jacket, black sash, and a white hakama. They are somewhat similar to what Ichigo's inner hollow wears. However, his jacket seems to have longer coattails than others, and the collar is rather high. Like most other Arrancar, he possesses remnants of his former life as a Hollow in his appearance. His Hollow hole is located on his sternum where a heart would normally be (though initially for some reason, the hole was located on the base of his throat; a change that was seen in both the manga and anime). The remainder of his hollow mask lies on top of his head, forming a broken helmet. He is the fourth-ranked Espada, signified by the tattoo on the left side of his chest.
Ulquiorra is a very cold, callous, dispassionate figure, and is rather aloof, brooding, and indifferent, willing to harm both his comrades and enemies should they ever get in his way. He refers to anyone he does not find interesting as "trash" and treats them as expendable. Despite this, he is not particularly violent, unlike most of his Espada comrades, and will only fight when provoked or ordered to by Aizen.
Ulquiorra has a strange habit of killing victims he is particularly interested in by stabbing them with his bare hand in the same location as his hollow hole. Whether he is consciously aware of this habit or not is unknown. During a speech to Orihime, he claims he cannot believe in human emotions, which he refers to as the "heart", reasoning that if his eye cannot see them, then they do not exist. These words, and much of Ulquiorra's overall behavior, can lead one to assume that he is a firm believer in the concept of materialism, which also connects to his aspect of death as an Espada, nihilism. It would appear that as a result of his isolated life as a hollow, Ulquiorra does not understand feelings and emotions as well as empathetic characters like Orihime tend to. His overall behavior towards his allies and enemies, as well as his apparently self-inflicted habit of stabbing people in the chest, may symbolize that fact. In the last seconds of his life, he seemed to have finally found his own "heart" and understand feelings.
His cold demeanor allows him to stay completely calm and in control in most situations, and he is not easy surprised or caught off-guard. However, he does not seem to comprehend the human trait of fighting against all odds or the very concept of a human heart/emotions; during his latest battle with Ichigo, he completely overwhelms the Shinigami after releasing his Zanpakutō, yet Ichigo continues to fight on regardless. This briefly causes him to lose his cool, causing him to shout at Ichigo out of frustration that "to continue fighting is pointless". He then transforms into his Segunda Etapa form in an attempt to show him "true despair". He also seems to contradict himself, telling Ichigo that it's natural for humans to mimic hollow to become stronger, but they will never be the equal of hollows, though the Arrancar are doing much of the same by imitating Shinigami.
Ulquiorra is also highly perceptive, cunning, and analytical; during his and Yammy's first visit to the human world, he makes several surprisingly accurate remarks on the humans who confronted them. He theorizes that Orihime Inoue's healing power is a temporal-spatial ability, which Aizen later describes as the rejection of fate, and comments on how Ichigo Kurosaki's Bankai can easily cut through Yammy's defenses. He also notes Ichigo's power fluctuation, which varies between very weak and stronger than his own.
Ulquiorra seems to be demanding as well, such as when he came to Orihime's chamber and ordered her to eat a meal an Arrancar servant brought in, claiming that, for Aizen's benefit, it was her "duty" to stay alive. When Orihime hesitated, he threatened to force the food down her throat, or strap her to a table and feed her via an IV. This also implies that, while he prefers not to dirty his hands, Ulquiorra is fully capable of committing truly abhorrent and inhumane actions without feeling any shred of remorse or hesitation.
After Ichigo's hollow form overwhelms and strikes him down during his last battle, Ulquiorra still maintains his composure and calmly berates himself for being defeated by a "human-turned-hollow". Believing that he no longer has a purpose in life, now that he was quickly defeated by his opponent, he then demands that Ichigo kill him, and compliments Ichigo when he decides to use a point-blank Cero to kill his opponent, claiming that the lack of mercy was "rather Hollow-like". This is a marked departure from most of his fellow Arrancar, who mostly died cursing their enemies or with an abject fear of death.
Source --> Bleach.wikia.com
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