"Animal behavior in a zoo is nothing like natural behavior."
However, some natural human behaviors can cause brief states of euphoria.
"But that would return them to their natural behavior, right?"
All natural behaviour has, therefore, become so by going through a stage of being unnatural.
I don't know what you saw them doing, but it could be a natural behavior.
After surgery, dogs are allowed to bark more freely, which is a natural behavior.
Matching the human's gaze is one way Leonardo seems to exhibit more natural behavior.
The natural behaviour would only occur if the creatures were completely comfortable.
Whenever possible, he wanted it to seem like improvised natural human behavior.
It allows the animals to feel more relaxed and encourages their natural behaviors.