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Molly first appeared with Danny in My Little Pony: The Movie when she first came to Ponyland when the ponies needed Megan's help to defeat the Smooze that was created by Hydia and her dimwitted daughters, Reeka and Draggle who plotted to rid of all of the Ponies in Ponyland.
Molly is often scared around monsters, but is never too scared to fight with Danny.
In the My Little Pony Annual 2013 comic story The Fall of Sunset Shimmer, Molly's name (and also Megan and Danny's) appeared in a flier for the Canterlot High Sundance. She's apparently a teacher who, along with Megan and Danny, handles submissions for the Yearbook in Room E.