In her initial appearance, Buneary is a cheerful and shy Pokémon and she has a crush on Ash's Pikachu similar to Ash's Chikorita when she has a crush on Ash. She is also became embarassed when seeing Pikachu until she cries when he tells her to take it easy. The two are soon friends when Pikachu is determined to save her as both teams up to stop Team Rocket. Buneary is also became good friends with Dawn after she was caught by her and still maintains her friendship with Pikachu and Dawn's Piplup.
Like Dawn, Buneary likes dressing up in beautiful clothes and shows her pretty side. She is also a kind and helpful Pokémon, such as helping to make Pachirisu feel better by giving her vest to it in Doc Brock!. When her friends are participating in competitions, she plays the role as an encourager. She and Pikachu are mostly seen cheering for Dawn whenever she enters Contests.
When Dawn reunited with Ash and met his companions, Iris and Cilan in East Unova, Buneary showed her shyness by hiding behind Mamoswine.
The moment Dawn saw Buneary in the episode Setting The World On Its Buneary!, she was determined to catch her due her cuteness, but failed due her lack of knowledge. At the end, Buneary expressed her crush towards Ash's Pikachu with her strange behavior towards him. Dawn managed to catch the Pokémon and Buneary was more than willing to go knowing she would travel with Pikachu by her side. This caused a Phione to fight against Pikachu, but Buneary decided to fight Phione. Phione was defeated and returned to its family.
Ever since then, Buneary was used a lot in the Pokémon Contests as well as in battle. As time went on, Buneary appeared to lose her romantic feelings for Pikachu. Despite her small size, Buneary was surprisingly powerful and was often used in battle as well as in contests.
In Piplup, Pansage and a Meeting of the Times!, she is pleased to see Pikachu again and Ash's Oshawott is surprised when Buneary goes for Pikachu instead of him, due to Ash's Oshawott having a crush on Buneary.
|Bounce||Setting The World On Its Buneary!|
|Ice Beam||Setting The World On Its Buneary!|
|Dizzy Punch||Setting The World On Its Buneary!|
|+ indicates this Pokémon used this move recently.*|
- indicates this Pokémon normally can't use this move.
- Tomoko Kawakami (Japanese role until her death)
- Satsuki Yukino (Japanese)
- Sarah Natochenny (English)
- Buneary had a big crush on Ash's Pikachu. Later, despite going separate ways with their respective trainers, when Pikachu and Buneary were reunited in East Unova, Buneary was shown still interested in Pikachu.
- When Buneary gets near Pikachu, she swishes her fluff on her legs as if it was a skirt.
- Buneary is Dawn's first Pokémon to be confirmed female.