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My recommendation would be to spend some time with a good disassembler. Find a bit of code to analyse that's big enough to be interesting and start adding labels and comments until you end up with a fully documented piece of code that you understand well. Then improve it. If it wasn't originally written in optimised assembly then optimise it. Rinse and repeat until you've reached the level you're looking for.
Another similar suggestion, if you're comfortable with C, would be to write something in C, make it feature complete, then find the handful of functions that are "hotspots" and rewrite them in assembler. You can even start with the compiler generated assembly to give you a working, if non-optimal, starting point.
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