Once you are satisfied with your building and have run out of places to glue on detail, you are ready to paint it. Personally I like to use Enamel based paints (like the flat Testors stuff) because it makes a better wash and the metallics are nicer, plus it is more resilient than water base paints. However, you must use paint thinner to make washes and to clean your brushes, so I don't recommend enamels to everyone.
Much like miniatures, a building is much easier to paint if you prime it first. Unlike miniatures, you want to prime in a dark color, ideally black. That's because the fastest way to paint a large object like a building is to drybrush it! You can buy flat black spray paint or primer from from a hardware or DIY store, or your local Games Workshop. Make sure you spray outdoors, and be sure to lay out a disposable drop cloth or newspapers to spray on. If your building has windows or holes, you'll want to spray the inside first. Be sure to get your inside surfaces fully painted so they don't show up from the outside (especially if you didn't add detail to the interior). This is easier to do if you don't glue a bottom on your building. Don't worry about getting every little crack and gap painted- if you put too much primer on, you'll start to gum up your details! Wait at least a couple of hours for the primer to dry. Now, fill in those little gaps and cracks that your primer missed with some thin, flat black brush paint. Once this is dry, you are ready to begin dry brushing.
Get yourself a few cheap, large brushes (even those nasty nylon bristle ones will do) with a head about 1/2 inch wide, and preferably a flat (not round) head. You only want the bristles to be 1/2 to 1/8 of an inch long, so if you need to, use a pair of scissors to cut your bristles shorter. This should make them nice and stiff.
To drybrush, load your brush with paint, and brush it against a scrap of cardboard or paper until it starts to thicken, and is barely coming off the brush. Now you can apply it to your model, rubbing the brush back and forth just hard enough that the paint rubs off on the high points of your detail. Be sure to test your brush before you paint your model-paint that is too wet will streak and smear, ruining the effect. If your brush starts to dry out, you can press harder, or just repeat the process of loading your brush. For best results, go "against the grain"- brush such that the bristles run perpendicular to your detail.
For your base drybrush, you'll want to use colors appropriate for a building-rust, blue, green, brown, or gray. You can even use different colors for different parts of a building (like rust for the bricks, blue-gray for the metal bits, and brown for the roof). Textures like mesh, grid, brick and corrugated metal drybrush best, but even smooth surfaces can pick up a bit of shading and color. You'll notice that the dark primer makes your drybrushing really stand out. You can drybrush a second coat or a lighter shade to really emphasize detail.
Now that you have some color on your building , you can make it even grungier looking by doing some washes. To wash, use a small, round brush, and mix up a small batch of really thin paint. (If you use water base paints, Inks work well for this). Soak up some thin paint with your brush, then just dab it onto your model. It will soak into the cracks, and will even streak downward quite naturally (if you hold the model right side up and give it a bit of help by blowing or brushing downward). Washes are great for simulating rust -use a reddish brown color around and below metal bits. You can also simulate grime and dirt with a dark brown wash.
To finish off your paint job, you can use some "detail" drybrushing. Wait for the washes to dry, then get a small drybrush ( about the size of a normal brush, preferably with a square head) and drybrush over small areas of detail that you wish to highlight. Use metallic colors like silver, gold or copper to highlight your metal details (rivets, pipes, plates). Use lighter shades to highlight the edges of your building (highlight brown and rust with tan, highlight blue with gray, gray with white). You can even use darker colors (dark brown) to simulate streaks of grime (under windows, around vents).
Now if you want, you can add transfers, decals, or stickers to your scenery. Use arrows, skulls, caution stripes, numbers, even blocks of text to make machinery look more realistic. To ensure they have a flat finish, apply a coat of flat lacquer over them after they have dried or are firmly attached. You can even make little storefront signs out of paper and glue them onto the front of your building. Now is also an excellent time to pull out that tiny brush and add small markings or even graffiti to your scenery!
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