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You use either one for different reasons.
Clay bar is to remove contaminants embedded IN the paint. This is a very gradual but gentle approach to removing particles that got stuck on the paint surface.
Simple Green is a degreaser that is best used for removing oily and greasy stains. I use SG on the underchassis, wheel wells and engine bay, sometimes on the wheels if brake dust is significant.
If you accidentally get Simple Green on the paint and have streaks of white marks, use paint cleaner to even out the color.
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