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That harbringer looks fantastic; I have no advice on how to improve because I think it's perfect like it is. I think the hardest thing about using necron bits is they make everything look necron right away! But the harbringer is subtle enough to take that appearance away so big thumbs up for that.
I also like the direction you went with the mastermind; my only advice would be to remove the halo on the servo skull and maybe add a bit more wiring. I feel like more skulls with more wiring would add a really nice flavor to the army, whether its dark in a chaosy sort of way or not...it certainly seems twisted.

All in all great army so far, this one takes the cake IMHO of your armies to date. Keep it up!

EDIT: in response to your query, I'd say that I would maybe steer away from using the tomb spyder body and go with something like the terminator torso to beef it up to hold bigger weapons. As far as weapons go, you could maybe mount some dreadnought-sized weapons or maybe convert some ork-imperial hybrids that would look exceptional (I'm thinking along the lines of those "count-as" boltguns you were using for the old knight titans).

I think they would work well as daemonettes; they look quick and deadly with a thrust of that tail blade. Their size and construction looks like it could warrant a very fast little critter. My only real advice would be making the spiders a little less necron-like, but if you like them just like that then I have no issues. Daemonettes would work great, especially if you're trying to get better CC punch

I think that updated harbringer looks great; you hit it right on the money. I don't think any other changes are really necessary, though I can understand why you might want to make some more adjustments to give it more of a "chariot" feel. Still, I give it a big

Have you decided what the steel scorpions will count as?