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Since the face mould needs to be redone as it is, might as well take this opportunity to change a few other things that were bothering me. One was that the "toon" look was getting lost and I attribute that to the level of fidelity of the facial features... especially the nose! Luckily I came across a toon nose I really liked by Dmytro Bajda. Shout out to him for his amazing work! I remodeled Aleysha's nose in a similar style. I think it looks much cuter and is getting back to being more stylized which is what the plan was initially. 
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The first version of the face cast was both a success and a failure. The face actually does fit onto the skull and the magnets hold it in place, but the casting method and the mould are very crude and the edges are dirty. Thin silicone walls caused air bubbles to get trapped in unfortunate places and when the mouth opens the skin is pulled away from the eyes so there will need to be more magnets under the eyes to prevent this from happening... there is a lot to be learned from this. The skin needs to have a certain thickness to look and feel right and not stretch too thin and let the skull shine through (even if it's not realistic). The next iteration will reduce a few parts on the skull and make the wire attachment mechanism for the jaw simpler as well. The best part is no part.  Overall I can see though that with a little better execution this might actually work.
After sanding and grounding and spray painting the skull a little it was time for a complete assembly. Everything fits well into place and the jaw articulates well.  For the assembly I got some 2mm diameter aluminum crafting wire (2x 4cm long pieces) and M3 stainless steel screws. The ends of the aluminum crafting wire are wrapped with black duct tape as I originally planned for 3mm diameter wire. But that turned out to be too tough to bend.  Here is a back view of the skull and the screws. The back of the skull is really rough as that's where all the print support structures were and I did not bother cleaning it up properly as this will be hidden in the joint between the skull face and the cranium part of the skull
Magnets have been glued into the back piece of the face mould. Magnet capsules have been inserted and the excess silicone trimmed off with nail scissors so no capsule silicone will stick out the front of the face. Ready for casting!  Decided to not make the face mould pretty on the outside and just focus on the inside. After all that's what counts when you make a cast. The rest just needs to work. Took long enough but both halves of version 1 have finished printing. It was a bit tricky finding a good orientation at which to print these two pieces with minimum support structures. The back of the mould was printed with a rougher setting to speed up the process and the front part of the mould was printed at the finest setting my ender 3 could muster so the surface of the face is as smooth as possible out the box as it's hard surface finishing concave shapes like this.  Next up some magnets need to be glued into that alien looking back part of the mould so they can hold the encapsulated magnets prepared earlier in place inside the mould.  These magnet capsules will then fuse with with the face silicone when it's curing and hold the face in place on the skull understructure later on. ... At least that's the plan. We'll see how it works out.
The printing of the skull face parts is complete. Magnets are glued in. Time to put a little surface finish on and fit it together.  More progress on the skull face. All magnet sockets and screw holes are now in place. Skull face, jaw and back plates to hold the jaw wire in place exist and should work for this initial prototype. Screws and crafting wire has been ordered. Time for a test print!  The skull is starting to come together. Worked out how I am going to attach the face, made most of the magnet sockets and screw sockets... now I just need to come up with a good mechanism for attaching the jaw and then make the mould for the actual silicone face.  Finally got around to casting the first batch of eyebrows, lashes, teeth, eyeballs... to test out all those moulds. The first attempt failed because the silicone was too viscous to seep into those tiny moulds using gravity alone. So for the second attempt I used a syringe to inject the silicone into the moulds. That worked really well but resulted in silicone being pushed into the gaps between the moulds so there was a lot of excess material that needed to be trimmed off afterwards.  Turns out cutting the excess material off is quite tricky with tiny, soft shapes like that. Not a very exact process at all. Will need to find a way to optimize this at some point. The teeth also have the seams in unfortunate places so might need to redesign that mould at some point to get it perfect.
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