The whole idea of nix/os is that the system resolves paths internally. Changing a wallpaper declaratively should be done by pointing to a file in your configuration. NixOS then will copy this file to the store, and point a symlink to it.
At best, this will just break quietly when the hash changes because a dependency of gnome updates, and at worst it will corrupt your nix store and brick your machine.
You should never ever manually edit the nix store!!!
To expand on this: you may not see any issues at first, but during the period of time where the nix store is mounted read/write, other programs (that are badly written and expect to be able to modify files where their program is installed) can silently edit files in the nix store and cause issues with your system. You also open yourself up for user error, obviously.
This method is like using a hammer to put a screw in your wall - hammers are for nails, not screws, even if the screw happens to go in - and is misinformation. Use the tools for the purpose that they are designed for.
To that end, I don’t use gnome, but someone else seems to have figured this out already:
Is the Nix way not straightforward? Do you do anything the Nix way? Will you do the next thing the Nix way? Nix was meant to be an alternative to such mutative workflows as the one you’re suggesting. And has been somewhat successful in that.