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Sit on top of a nuclear weapon, and detonate it.

Nothing faster, period - and no time for pain impulses to travel along nerves either.

A block of C4 would do the same. Also faster than nerve impulses. In fact dropping off a building on your head would be faster on impact. Nerve impulses are slow.

Well, "fastest" along with painless was specified. The prompt gamma rays from the nuclear blast would kill all tissue within a very small fraction of a second - much faster than the comparatively slow C4 shock wave. :-)

In practical terms though, not much difference. If practicality was the major concern I'd say a 12-gauge discharge using #2 shot or so through the forehead angled down towards the back of the head would work well. Messy cleanup, but quick and painless for the deceased.

These are all very impractical methods --- there is almost zero chance of this happening unless you somehow manage to get your hands on a nuclear weapon as a private citizen

The question did not specify practicality as a requirement. The request was for "fastest and most painless" only. :-)

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