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What is the best caster to go with Mechanithralls, Necro-surgeon and stitch thralls?

If you look at the mechanithralls you can see that they are brilliant at killing what they hit. Either two POW 11's or a single POW 15 is good at killing a load of stuff out there.

Their issues are with landing those hits in the first place and surviving with sufficient numbers to get to the enemy. So we can look at casters that can help in these categories.

Deneghra1 or 2 are the queens of debuffing the enemy. Cast those spells at the enemy and let the mechanithralls do the work.

Skarre1 deserves a special mention as Dark Guidance is a mean spell for mechanithralls and her feat lets them hit even harder. POW 20s on the charge. Then ARM 17 lets them survive the AOEs that could come back.

Gaspy3 is a similar caster with slightly less ability to get the mechanithralls up to massive levels of damage but more constant during the game. Ashen Veil will also help them get to the enemy.

Scaverous is a good caster, just pushed to one side by the Deneghras. Death Ward can be helpful though and Icy Grip again helps the mechanithralls hit the enemy warrior models.

The other casters will have their own benefits but I've looked at the ones with the most complete solutions to the mechanithralls issues.

Is there a caster that has the best synergy with a tier list?

Don't take a theme list.

It looks like you are a new player and as such a theme list will restrict you far too much when you should be experimenting with the entirety of the faction. Theme lists can be a good thing but generally you give up a lot of freedom for very few benefits.

Those casters I have listed are good options for a new player, each with their own style. Find their models and see which one you would prefer and play that one. Just not as a theme list.

I have been steering away from the theme list for that reason.