In After Effects I used SA Color Finesse 3 UI, which allowed me a full interface of controls to edit the colour of my image. I found this gave me a wide range of control, especially with being able to individually control highlights, mid tones and shadows.
There is also a split screen option that allowed me to see the contrast created, and play with how far I could push an image.
After Effects also allowed me illustrative control through the form of masking. As mentioned, in reference to The LOTR Fellowship video, selecting areas and highlighting/adjusting them gives further control to the overall scene and can bring forward a performance. I found by masking and tracking the face of my actress I could stop the colour grade of the image from seeming overwhelmingly contrasted and unnatural.
I also edited some footage in Premiere Pro, this was initially to get a feeling of the tones I overall wanted to create but some of the footage ended up being colour graded completely by this process. There is less control this way, but drastic results still can be created. By using curves I could create contrast and give my images a slightly 'unreal' look.