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Great Grandma Harriet is a minor character, and part of the Loud family. She was first mentioned in "Changing the Baby", and again in "Snow Bored". She is deceased, as Lucy speaks to her "ghost", and she makes her first physical appearance, albeit in a photo, in "Spell It Out".
Not much is known about her, except that she's a deceased relative of the Loud family. Lucy still treats her as a living person, which indicates that, (assuming Lucy and her siblings knew her when she was still alive) she and Lucy were very close.
In "Tea Tale Heart", Lucy finds a doll in one of Great Grandma Harriet's trunks in the attic.
When Harriet was a child, she bears a striking resemblance to Lucy, with a few exceptions: Harriet was seen wearing white pearl earrings, a pearl necklace, a black dress with a brown waistband and brown cuffs, and a brown 1940s hat, as opposed to Lucy's outfit.