Can you change selection keys?

I would like to change selection key:

Ctrl+Shift+Left Mouse

(polysurface/surface faces, edges, boundaries, mesh faces or edges, and objects within groups)

Is this possible?

Change that key combination to something else? No, I believe those settings are hard-coded.

Yes

To: Ctrl+Alt+Left Mouse would be better….

Ctrl+Shift are to close, I use it a lot when SubD modeling in Rhino7WIP