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I wanted a sleek, otherworldly look for my necrons, I painted a couple of the features green, the inner crevices a black/green mix, gold for the spinal/random bits, and made the armor a black, glossed over. How do I keep that look, while also highlighting it?

You've a couple options. Seeing as you already put the gloss coat on, your best bet is to leave it as is and let the gloss do its work. Adding highlights on top of it will look bizarre and most likely worsen the effect. If you actually want to paint the highlights it's better to start over with solid matte black and hand paint your highlights. Look at some images of gloss black surfaces and shapes. Look how light reflects off objects. A believable gloss black is not a basic effect to achieve, but just takes practice.

Hope that helps
BB

Generally, you don't. High gloss finishes reflect light so readily that illusory lighting effects (i.e. highlighting) at best get washed out and at worst actively conflict with those reflections of ambient light. Basically, the sheen highlights for you. Better to gloss an even coat of color (as you've already done) or use a matte or satin finish over painted highlights. At least in my opinion, the two don't mix.

You could also try undercoating grey, heavily washing black to give some natural highlights and shadows, then using a gloss varnish over the top.

I can't really see a way of highlighting an already glossed paint without adding another layer of gloss over the top, and I would never paint anything straight black as it is a pain in the butt to highlight and shade.

airbrush on some highlights and use a gloss varnish as your thinner.

Very sharp highlights, tightly constrained. Gloss at the end.