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I've been using the Split Toning functionality of Lightroom and Adobe Camera Raw for some time now -- you can see the effect in this video.
How would I go about performing adjustments like these in the core of photoshop? Note: I don't want to do this on a grayscale image, I want to adjust the hues of the shadows and highlights of a colored image.
Image > Adjustments > Color Balance
will get you close. It's not as simple as a hue and saturation slider, but it does allow for color adjustments based upon shadows and highlights.
You could always use Filter > Camera Raw Filter from within Photoshop as well. Split toning is part of that filter.
Use the "select > color range" tool with the highest fuzziness value. Select a dark tone somewhere around "75% grey."
Hide the selection so you can see better, and use "image >adjustments>selective color"; make adjustments to "neutrals" only. Adjust saturation and/or levels as needed.
Deselect and then repeat using "25% grey" tone selection.
(Control + U) on Windows or (Command + U) on Mac will bring up Hue/Saturation panel. In this panel you get similar controls to fiddle with. Using a pair of layers you can achieve the desired results.
