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A 'legendary' Bioni-Spirit is any Spirit that has over 200 FE. They are sentient, unlike most lesser Spirits, and usually have some sort of important role to play in the universe. Legendary Bioni-Spirits all hold immense power.
The Nui
Avohkii-Nui and Kraahkan-Nui, the most powerful Bioni-Spirits and master of Light and Shadow, respectively. According to legend these two were created at the same time as the Bioni-Lords universe, and ever since they have been battling each other in a pocket dimension with no way to escape short of killing the other. Legends also say that all Bioni-Spirits serve either the Order of Avohkii or the Order of Kraahkan, with "sub-Orders" led by the Hapori.
The Hapori
Four extremely powerful Spirits who take varying positions in respect to the world. Hapori Tohu and Hapori Dume assemble members of their Orders and wage war against one another, making them seem similiar to the Nui in a way, while Hapori Gahu and Hapori Zadakh seem to take very passive roles.
The Gahu
Nine Spirits who have the ability to shapeshift into a multitude of other Spirits, their own unique Spirit form, a human form, and a specific animal. They make up the Elemental Ring of the Order of Dragons, save for Gahu-Shadow who defected and began gathering the Dark Knights. The Gahu were created by the First Element-Lords, who needed to release some of their energy to stabilize their bodies.
Twilight Guardians
Three Spirits called upon to keep Light and Shadow balanced. They include Hyper Sonic, oriented with Light, Metadon, oriented with Shadow, and Cuerveracios, oriented with Twilight. Their pre-upgraded forms are thought of as Sub-Twilight Guardians, but don't handle matters as important as those given to the Primary Guardians.
Vassal Class Legendaries
This class includes the Four Elemental Knights, One Winged Angel, Tabuu, Atomicus, and Legolord. Each of them has served one or more of the Gahu at one point in time, hence the term "Vassal Class."