Is there a way to setup Gimp to use a held key (e.g control or alt) to do the same as mouse click?
3 Answers
The general answer is no.
There are some mouse clicks in the tool boxes and editor dialogs which change parameters (like brush size) - these are mapped as "actions" inside GIMP and you can create keyboard shortcuts for them (including using the F keys) under Edit->Preferences->Interface->Edit Keyboard Shortcuts...
But probably that is not what you want - the main mouse button-click effect in GIMP is stroking the image with a paint tool - and that is wired in a different way inside the program: it can't be replaced by a keypress.
However, there are different painting devices that can be used that might serve your needs - a graphics tablet like those sold by Wacon provide a fundamentally different interface than mouse not just for GIMP, but for all drawing programs.
And GIMP is somewhat a unique program that can actually make use of a MIDI controler (like a MIDI foot controller) to control the pressure of the painting - so, if your problem is getting rid of the "click and hold" action for painting with the mouse, a proper configured such peripheral could serve you.
That said, this question would be ontopic for https://graphicdesign.stackexchange.com/ and is offtopic here - I hope someone can move both the question and this answer there.
If GIMP does not allow such function. I have a suggestion, if you are using Ubuntu you can enable mouse control by numeric keypad as explained here. After enabling mouse control by numeric keypad you must turn Num Lock ON and press the key 5 to simulate a mouse click.
One workaround I use is to rebind an unused key to left mouse button, through macro or some other method.

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