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Hitsugaya is generally mature and serious, in contrast to his free-spirited lieutenant, Rangiku Matsumoto. Despite their personality differences, he and Rangiku seem very close. Tōshirō is shown to be easily annoyed by others goofing off or drawing unneeded attention to themselves, as shown when he leads a team of Shinigami into Ichigo Kurosaki's school.[4]

Hitsugaya hates anything that he deems childish as well as being described as something close to a child, such as an elementary school child, a further contrast to his appearance. This is shown more in the omake chapters of Bleach, such as the short comics in VJump and the sand castle contest chapter released along with Chapter 238. He is also mistaken for a kid in several of the omake chapters, much to his annoyance. During the ending credits of the Sealed Sword Frenzy, he is in the human world and dressed in a young boy's school uniform, and Hinamori has to pull him out of hiding. He is overly protective of Momo Hinamori, due to the fact that they were old childhood friends. Hitsugaya dislikes summer and warm weather in general.

It is also known that Tōshirō's favorite food is amanattō. His grandmother even occasionally sends it to him into the division quarters. He does not like dried persimmons. Back in his childhood in West Rukongai, he was so skilled with spinning tops that he became the local undefeated champion. He works very hard, but his motive seems to be that if he finishes quickly, he can return to his afternoon nap. He believes in the saying "children who sleep well, grow well," and hopes to grow quickly, a wish shared by his subordinates. Naturally, they do not voice this fact in front of him, for even regularly practicing this adage for so long, he didn't really grow in height.[5]

Hitsugaya is usually joked about by many of the other Shinigami in Soul Society as well as by his enemies. Despite these jokes, or perhaps because of them, Hitsugaya has developed a cold attitude toward most people; he tolerates these jokes and goes on with his duties. Although he has shown anger toward jokes, he doesn't take action against whomever insulted him unless they are his enemies, but has never overreacted because of them. The only thing he can't tolerate is not being addressed as "Captain Hitsugaya," or an inappropriate use of his name, as he worked very hard for the title so he gets angry when not addressed as such. Coincidentally, though, he does not address any other officer with their title, only their last names. The only people that actually call him by his given name are Ichigo, who is constantly reminded to address him properly, and Hinamori, who is the only person allowed to get away with it. Hinamori tends to call him "Hitsugaya-kun" and both she and Ukitake occasionally use "Shirō-chan" (シロちゃん) — a nickname meaning "Whitey" (Snowy in the English manga) in reference to his hair — in both cases without any repercussion. In the Shinigami Golden Cup sketches (omakes found at the end of episodes of Bleach), Jūshirō Ukitake comically gives Hitsugaya candy and other food because "Jūshirō" and "Tōshirō" sound similar and because they both have white hair, making them both "Shirō-chan." The first character in Hitsugaya's given name, Tōshirō, means "winter," which is appropriate given his white hair and ice-type Zanpakutō.

During his duel with Gin Ichimaru in the anime, Ichimaru remarks that Hitsugaya is the embodiment of a heavenly guardian that would be reincarnated every few centuries. This is attributed to his given name Tōshirō, which literally means "son of the winter lion" (dragon/metaphor for magnificence).

Even though he has relatively little amount of interaction with Ichigo, he helps in several potentially disastrous events, whenever ordered to by Yamamoto.