Ultimately, "better" and "good" will be seen in retrospect, or in realizations that things are WAY better than they used to be. That "better" is between children and parents, and happens when it happens, not because of anything anyone here says or thinks.
"I read for them as needed, then suddenly I realized they were reading these things without me. I've been amazed at how quickly reading progresses when they're ready — one of my kids went from barely reading to reading Harry Potter and the Little House books in what seemed like overnight."
If budding unschoolers will look at how they learned things outside the classroom, and use that as a model and a goal, that helps. They don't really have to hunt down other unschooling families, although it doesn't hurt. A family isolated from other unschoolers might do well to brainstorm examples of things they've learned informally and naturally, and to look around for other people learning things in the same manner.
It's sweeter to say yes several times a day, with the option to still say "not yet," than to have one big "anytime, anywhere" that then might need to be amended.
[But she's asking even though I've told her she doesn't need to ask.]
There are times it won't be a good idea. Say yes, sweetly, when she asks, instead of correcting her and making promises you might not be able to keep.
Connections and parodies, comparisons and contrasts—learning is all about seeing what is like what, and how an image, idea or object can apply or fit where.
Don't be afraid of happy connections and rearrangements. Rejoice!