If you like the sight of colourful brake calipers peeking out from behind a set of rims, then make sure to tip your hat to fuel injection and catalytic converters. Painted brake calipers came about in the 1980s and 1990s as a result of aftermarket wheels, which came to prominence largely because car enthusiasts either couldn't figure out of to deal with fuel injection or couldn't legally tamper with emissions equipment. Regardless, the trend took hold and is now an integral part of any hot rod or custom's design scheme.
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Brake calipers get very, very hot; hot enough to destroy most types of conventional paint. This, combined with the calipers' exposure to brake fluid and road debris, necessitates some very specialised paint. It you're looking to just hide a set of calipers behind the wheels, then you could go with a flat black spray-on barbecue grill paint. Engine enamel will also last for a while, but your best option is a specialised ceramic-enamel. Use the brush-on paint; it'll go on thicker and will likely last much longer than any spray paint.
You can paint the caliper on your car, but removing it will make for easier cleaning and painting. Cleaning is essential, since any kind of oil, wax, grease or brake fluid on the caliper will create kill paint adhesion in that area. If you're looking for a fully professional job, then disassemble the caliper, send it to a machine shop to have it hot-tanked, clean it with alcohol when you get it back and then paint it. This will also give you an opportunity to perform some preventive maintenance on the slave cylinder and replace the pads.
Porsche and Ferrari were two of the first companies to integrate painted brake calipers as a styling accent, which is why the first brake caliper paints generally came in bright red, bright yellow and black. Nowadays, brake caliper paints come in dozens of different shades designed to match any paint scheme. Don't be a slave to convention; remember that your newly painted calipers will become one of the most visible aspects of your car's external styling, so stay away from those traditional shades if they don't match the rest of your car.
Powdercoating is another option. Powdercoating involves spraying the caliper down with powdered polymer paint and baking it on in an oven. When the polymer dust melts, it'll form a solid shell over your caliper and leave a smooth and flawless finish. Powdercoat comes in nearly any shade that you can imagine -- including chrome and black chrome -- and will far outlast almost any kind of enamel paint. This is especially true of ceramic-based powdercoats like those designed for exhaust headers. But use caution; those ceramic-based powdercoats are designed as heat insulators, which is the last thing you want on a brake caliper.
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