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[Vector]

Vector, with the no-highest-side method, what kind of irregularity problems will I get?

Depth issues.  It is extremely hard to pour candy to a perfect level without getting it too high or too low, and then there's the fact that it's likely to have some weird bulging/pitting effects due to adhesion/cohesion if you get it any lower than perfect.  Any higher, and you'll get the bulging + a fringe you have to shave off.

[Cheddarius]

Can I pour a little extra, then skim off the top with a knife before it cools?

[Virex]

You could try. I don't know if candy's durable enough to machine it afterwards, otherwise you could just grind away any irregularities, since this techniques seems to be the same as metal casting and that's how the usually do it. To bad sugar caramelizes before it melts, otherwise you could have powder cast it.

[Vector]

Can I pour a little extra, then skim off the top with a knife before it cools?

Ooh, that's a good idea.  You might get streak marks, and you'll definitely have to do it pretty quick so you don't end up with a sort of wave, but that sounds like it might work.

On another note, how are you planning on removing it from the mold?

[Cheddarius]

...oh.
I hadn't thought of that.
There are solutions, but all the ones I can think of seem too complicated to be better than other methods.

How about this?
I make two identical half-molds, one the bottom and one the top, and fill them with candy. A little more than you need to fill the mold. Then I press them together, fitting them to each other, and squeezing excess syrup out the sides. I can just break/file that off later if there's a bit of residue.
If it's too hard to align them, I could make a hinged one... would that work?

[SirHoneyBadger]

I'm not sure about the moulding itself, but if you find something that will make good moulds, a lot of antique stores have really nice costume jewellery, usually for a great price.

[Vector]

If it's too hard to align them, I could make a hinged one... would that work?

Harder with hinges, because the hinges will get all gummed up.  Use a flat surface like a table or counter to align your halves.

I'd actually do what Pathos suggested, though, and let the two halves set (scraping them first) before adding a touch more mixture and pressing them together.

Not entirely sure--I'm mostly playing this by ear.  But it seems like your best bet.

[Cheddarius]

Hmmm, that sounds like a good idea. So add some more, press them together, scrape around the perimeter to remove excess glue. Excellent!

I'm not sure about the moulding itself, but if you find something that will make good moulds, a lot of antique stores have really nice costume jewellery, usually for a great price.

Hmmmmm... I'm looking for something really specific, so I don't know about that. What about baked sculpting clay or something for the positive?

[SirHoneyBadger]

It seems like clay might work, if you bake it. Worth a try, anyway. Just be certain that it's non-toxic. In other words, buy the clay from someplace reputable, and check the label.

Also, since you're making "jewels", keep in mind that the slower a crystal medium developes into actual crystals (crystallizes), the clearer the crystal will be. That should hold true for candy, too, I would think.

[Cheddarius]

Hmmmm, hmmm, interesting.

[Strife26]

I'm not sure how well that'd work, molten hard candy is like, really really hot. You'd have to be super careful trying to press anything together.

[Duke 2.0]

I'm not sure how well that'd work, molten hard candy is like, really really hot. You'd have to be super careful trying to press anything together.

It is hot, but even when really melted it is very thick and sticky. I'm sure a drop or two would work fine.

[Cheddarius]

Hmmmm. Well, I won't use that much, it'll only be between the two pieces. My hands will be at the ends, not actually near the thing...
Regardless, if it doesn't work, I'll see if I can maybe do the one where the top is open. Except I'll tape the two pieces together, and after the candy hardens, I'll take them apart.

Is it possible to melt down hard candy and reuse it? I'll probably have to make a big batch, and I don't want to waste most of it on a small experimental batch...

[Virex]

I'm not sure how well that'd work, molten hard candy is like, really really hot. You'd have to be super careful trying to press anything together.

Using a ceramic mold (Clay or plaster. Plaster's probably the easiest, though I don't know if it'll leave plaster on the candy), and towels to prevent spills from burning your hands it should be easily doable.

Also, depending on the mixture it might actually become amorphous instead of crystalline, in which case cooling fast would prevent it from becoming semi-crystalline, and preserving it's optical properties. Gut feeling says that full single-crystal crystallization takes far to long to be practical, so you'll likely end up with a polycrystalline or amorphous candy anyway.

[piecewise]

Ceramic with the correct glaze to make it smooth and non-porus would work but metal works best. I linked to that site for a reason, because it is probably going to be the very best way to do it.  To get a high quality reusable mold you're going to have to at least use kiln fired clay which can be done if you happen to have a friend in an art school or program. Even then its easy to break and not great at holding perfect shapes very well. Metal is the best, cleanest, safest solution. If you look around you'll find sites that do custom machining for relatively cheap, especially with simple geometric objects like what you want.

That, or you could just use these