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Depends what you mean by "hardest". Hardest to get a smooth coat is one thing, hardest to make look good is another.

Yellow is probably the hardest to get a smooth coat on. But if you're struggling, try to use Averland Sunset as a base. It's how I paint pretty much all my yellow now, makes it much easier. 2-3 thin coats of Averland Sunset will cover black pretty well. If you can use white as a primer it helps as well, but IMO if you have a black base it's not worth the effort of painting it white first and then painting it yellow, just paint it Averland Sunset and be done with it. You can also base brown.

Hardest to actually make look good... I'd have to say grey. It's really hard to make grey look good IMO. Other colours you can choose to either contrast different colours OR you can simply go light to dark and get a lot of contrast within the one colour. But grey, I dunno, I just find it really hard to give it the level of contrast I want and it never turns out looking how I wanted it to look.

 SharkoutofWata wrote:
And I'm just getting into Alaitoc Eldar... Yellow helmets on a black base coat and blue layers and no painting skills to call my own. I'm gonna be screwed.

Seriously, Averland Sunset

Do the black basecoat, 2-3 thin layers of Averland Sunset with a nice large brush, highlight by mixing in a bit of white and that will give you a dullish yellow. If you want to make it a bright yellow, hit it was a yellow glaze.

This is similar to how I have been doing some of my Orks, these were black base, 2-3 coats of Averland Sunset for the flames, and then paint the flame tips in orange then I spent a bit of time blending the orange and yellow together. The take home message is that even from a black base it was pretty simple to do.