Natural light works great for portrait photography, but if you want beautiful results, you need to understand the types of natural light to use - and the types of natural light to avoid. Some types of light will create soft, beautifully lit portraits, while other types of light will produce harsh shadows, unpleasant highlights, and just an all-around bad effect.
I'd recommend working in open shade, which you can find under awnings, at the edges of trees or buildings, and inside doorways or windows. The idea here is to position your subject in an area that's shaded, but not too shaded. You want the soft, flattering effect that's produced by shade, but you don't want to work in heavy darkness.
You can also work in the evening, starting about an hour before sunset. The soft light of the setting sun will produce a beautiful golden glow, and you can often use careful side light.
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