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I'd like to see keycaps made from the following materials: ¤Borosilicate Glass (In various, but always translucent, colors; aesthetically akin to sea glass ¤Various TPE's (Thermoplastic elastomers) with a soft, "grippy" feel ¤Exotic plastics (polyolefin) such as UHMWPE, Zylon, PTFE ¤Acrylonitrile styrene acrylate (ASA)- while structurally similar to ABS, it's superior in every way including UV resistance, impact resistance, abrqsion resistance, etc. ¤Geloy Resin and Noryl GTX resin. These can achieve some amazing aesthetic properties including metallic and pearl flake metallic surface finishes that look exactly like metal ¤Keycaps treated with various "soft touch" polyurethane coatings
Mod keys would get my vote
Metal keycaps are fun! A big part of their appeal is the extra weight. They make a solid, satisfying 'thunk' when they bottom out - a much nicer sound than the plastic 'click'.
I've bought a small set of electronic scales so I can measure and compare the exact weight of different keycaps. Fun fact: zinc actually has a higher atomic weight than iron. So zinc keycaps are probably the heaviest practical ones.
There's a different tactile feel as well. Metal keycaps are smooth and cool, and pleasant to the fingertips.
The backlit/doubleshot ones are the best, in my opinion. Engraved legends can be difficult to read.