some Crown Chakra Thoughts,

[Plenum]

Is seeking alignment with the Crown the most worthwhile kind of work one can do?

I'm not sure one can be in alignment (or for that matter, out of alignment).  That's not the role of the Crown center.

Or is experiencing what is unlike the Crown what yields most fruits?

again, my understanding of the Crown center is that it's a repository or a source.  It represents the 'greater self'; which is still in motion, unlike the Higher Self, which is somewhat static and perfected.