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OK, I've been bitten by a rather sizable bug.

After living with an Imperial Knight player and reading The Master of Mankind, I have the urge to add a single knight to my Adeptus Custodes.

I love the background to House Vyridion, and I like the aesthetic of Knight suits that are paintless, salvaged, pitted suits, devoid of kill markings, pennants, and with only a tilting shield painted by the Scion piloting the suit.

It really clashes with the glittering gold and vibrant red of the Custodes.

BUT

How do you paint grey chunks of plastic as grey chunks of adamantine, without looking like you haven't done anything?

The way I'd approach a Knight like this would be to get a handful of different metallic paints, a couple of silvers/metals, a brass/bronze, a gold, maybe a copper too. Hit the main bodywork with a silver of your choice. A dark gunmetal is always a good start. Then do different areas different shades of silver to represent the scavenged nature of the warsuit. A leg might be a lighter silver as it's come from another warsuit. Part of an arm might be a brass plated donation from another household. Hit any pipes with copper. Maybe copper pipes are cheap and since it's a thrown-together salvage job, the pilots needs to keep things cheap and replaceable.

Another way to add some visual interest to what otherwise might be a huge chunk of metal would be use different coloured washes. A couple of coats of Nuln Oil will really darken just about anything. Sepia or brown washes can help age metallics really well.
Blues are also a good way of differentiating metals.
Whether could also be used to help break up a sea of metal. Scratches, dents. Acid scarring. Heat stress on weapons. Sooting on exhaust stacks. If it's got a chainblade, blood splatter is always an option.

There's plenty of cables on a knight just crying out to be painted red or blue or hazard striped.

I would recommend looking at how Iron Warriors paint schemes work - as Snrub explained using washes and different base layers will really help. You're relying on the texture to differentiate it from an unpainted surface.

So I might start with say Iron Warriors base paint, hit it with some Nuln Oil, light it up with some lighter metallics and then maybe drybrush some grays to cut the shininess of the metal.

You could also use weathering powders afterward to add some rust or dirt.

I would start with a dark-ish gunmetal over black heavy drybrush. Then a lighter drybrush of a lighter silver to bring the detail up.

Then you want to wash it with something to make it look a bit grimy - something like agrax earthshade maybe. Then hit it with a bright silver but only on the most raised edges and recent battle damage. This gives it the illusion of depth that is important for making tiny things look big and also highlights detail with some visual interest.

I would also pick some parts out to be different colours maybe like black or something or some brass/bronze fittings just for visual interest. But not in a paint scheme way - just like, this strut is made of ceramite so it's black, this bolt is a bronze colour because of the alloy it's made from, and so on. Don't go overboard but do a bit.

A very slight amount of rust-weathering might also be appropriate - I'd use a texture paint like dark brown rust and then sponge on some bright orange rust lightly over top, but I'd use this very sparingly on an Imperial model.

Would making a lower leg, or part of an arm Martian Red work? Perhaps a faded cog?

This implies that the Knight was once part of a different House and was destroyed and rebuilt.

If you have the skill you could drill into the suit and have battle damage/bullet strikes...

 Quixote wrote:
How do you paint grey chunks of plastic as grey chunks of adamantine, without looking like you haven't done anything?

You already figured out part of the secret: don't' paint the panels metallic. The key to a good piece is contrast, and so you'll need to push your two pimary colors: flat neutral grey and gunmetal, in different ways to maximize the effect.

The metal is easier, you can just use very subtle rust effects to push the grey warm. I wouldn't go full on junkyard rust (unless that's what you're into, in which case go get it), but rather some dots of rust at rivets and joins, and then some streaking down over the armor. If the trim is warm, I'd push the main panels cooler. Look at a payne's grey, or the Fang, or Mechanicus standard grey. You can't really wash the panels, unless you use oils as a filter, but you can layer up a little bit with brighter greys that are cool, like Dark Reaper. Alternatively, you can do burnt black metal trim and a warmer grey armor panel, and basically treat it like Imperium wraithbone.

Then, you want to pick out the details to pop. maybe find some metal to paint bronze (with or without patina), paint some cables in a burnt red, etc.