I've tried Debian, Ubuntu, Fedora, openSUSE, Slackware and Mint, but not to the depth of having attempted to customise just about anything which can be customised, so I don't know. Maybe another distro I haven't tried?

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The distro really has absolutely nothing to do with aesthetic customizability. Aesthetic customizability instead has everything to do with your windows manager, be it GNOME, KDE, Xfce, LXDE, or any other, including one that you could create yourself.

If you mean "customized the most through a GUI," then I'm honestly not sure which one is better. But if you mean "customized the most through any means possible," then the only limit to your imagination is the limit of your coding ability, no matter which windows manager you choose.

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Probably ArchLinux, not because it has a better gui but it doesn't have any. Yet you must not forget that to customize something you need to know nearly everything about it.

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