In her initial appearance, Buneary is a cheerful and shy Pokémon and she has a crush on Ash's Pikachu similar to Ash's Bayleef when it has a crush on Ash. She is also became embarrassed 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 also became good friends with Dawn after she was caught by her and still maintains her friendship with Pikachu and Dawn's Piplup.
Buneary also defends Pikachu from a wild Phione when the former had a crush on her and became jealous towards him. She volunteers to fight it in Pikachu's place. Once they clash with their Ice Beam and defeats it, Phione sadly said goodbye to her before leaving which shows its rejection.
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. She also likes Paris' Lopunny when they first met because of their evolutionary relation and became impressed to her beautiful side and its accessories.
When Dawn reunited with Ash and met his new companions, Iris and Cilan in East Unova, Buneary showed her shyness by hiding behind Mamoswine but she maintains her crush towards Pikachu upon their reunion.
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 but she still maintains her crush towards him. Despite her small size, Buneary was surprisingly powerful and was often used in battle as well as in contests.
In Arriving in Style!, Dawn and Buneary enter the fashion show along with Ash and his Pikachu as requested by the superstar Poké Stylist, Paris and her Lopunny which is Buneary's evolved form who is revealed to be the judge of the show along with the editor in-chief, Hermione. As the award is about to be ready, Team Rocket intervenes after Jessie wasn't pick as one of the runner ups due to ruining James' makeover from her and Wobbuffet as they attempt to steal all the unique accessories. It was stopped by Buneary's Dizzy Punch while Piplup does the same but fail and it was caught in a spin before it was saved by Paris' Lopunny's Hidden Power. Altogether both Dawn's Buneary and Paris' Lopunny use Bounce to knock the robot with a flying kick and blasts Team Rocket off in an explosion.
After that, Ash wins the Unique award with Pikachu and Paris declares Dawn and her Buneary is a champion making the celebrity Coco failed. Buneary hugs Pikachu for their win and both Dawn and Buneary give tiaras by Paris.
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.
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- 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.