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I have painted the majority of my Tyranids now, but I have left the winged models (Gargoyles, Flyrant, Hive Crone) because I do not know what colour to do the wing membrane in. I want to start painting these guys next week (hopefully have 100% of the army painted by Christmas). Across the Tyranid range I have used a consistent palate:
* The external rib-cage area is dark blue, with a grey-blue highlight on some models.
* The limbs (arms, legs, heads, tails) are turquoise, with a blue wash and pale-green drybrush.
* The carapace and claws are orange, with a red wash and yellow drybrush.
* The gills and eyes are red, with an orange drybrush.
* Models with fleshy sacks (eg Barbed Stranglers) are an off-white.
I have examples of all my completed models in my gallery here.

For the arm/finger parts of the wings I will keep the turquoise, and I will add orange to any claws on them, but I cannot decide what to do for the wing membrane. What would be a good colour to use alongside turqoise and orange?

I'd match either the limbs or fleshy sacks.

I'd go with a lighter version of the blue colour.

My two teef.

I'd actually go darker blue as I think it would look the best, however, it would make the most sense to go lighter blue than the limbs--thinner skin, light passes through.

I had not considered blue!

I have seen a technique of starting with a white base then layering washes to gradually build up colour. Would that be a good choice for, as Gordon said, creating the effect of thinner skin? Alternatively, would I be better advised to just use a lighter blue and paint as per normal?

You could do it either way, but with large surfaces washes can tend to look a bit splotchy if you aren't careful about pooling. I would recommend layering from light to dark and maybe a final light wash to tie it together. Or you could base in darker and drybrush lighter in the middle where it would be thinner. Check out Striking Scorpion's tutorial on YouTube on how he does his hive tyrant wings if you want to see an example of the latter.

Splotching on wings may also look pretty good.

I have three sets of wings I need to do at the moment, my flyrant I am planning on painting the skin of the wings white, then airbrushing a blue wash, then using a patterned mask to airbrush a blue over the top

I go for leather or skin look as the membrane of the wings is usually a stretched colour that compliments the skin.

If you want to get a wash on there without it looking too splotchy, i really do suggest a good coat of Gloss varnish (applied via airbrush) to give the wash a smooth surface to run into. Also, if using GW washes, get a Flow Aid and thin them down a little... maybe 2:1.

Check Tyrants and gargs in my gallery. This is exactly what I did and then a final light airbrush over the top to blend it in.

Hope that assist with the application of whatever colour you choose.

The blue gw glaze could look quite nice too, guilliman glaze i think then a coat of lahmian over that to make it matte but i definitly think blue would be best

Hmm... it sounds like this would not be the best situation to try and learn a new technique with. I may save that for an easier model in future and just use layering and drybrushing as usual (with a little wash into the edges).

Thanks for the advice. I think I have a solid direction now!