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Song 1: Renai Circulation; Kana Hanazawa
First of all, fill the lineart with a light base color.
Now let's add some shadows on a new clipped layer (to clip it, click the "Clipping Group" thing upon the layers board)
Choose a darker color and start painting with the Marker Tool.
Italy's hairline is pretty uncovered. His bangs cast a shadow on it and they're not so straight, so play with the colors in these tricky places.
Each hairstyle is different and needs to be studied and imagined at the sun, so you'll be able to put the right shadows on it.
Play with the pressure you put into your Pen to make darker/lighter shadows.
There not so much to say about this part. The only tip I can give you is to look carefully and imagine where the light will touch the hair.
Example: Look carefully at the left part of his hair. As you can see, there are some shorter tufts that stand a bit higher.
This height difference is important! What stands higher, will be lighter since the Sun will touch it directly.
The tuft below the higher one will be darker (in its upper part mostly) cause the small lock of hair above casts a shadow on it.
This same reasonig goes for the rest. Hair is made of tufts, isn't it? (:
Take your time: if you're not used to this kind of coloring, it could be tricky and not so easy to do.
Now, as always, adjust Contrast, Luminosity, Color and things like these to make it look better~
Here comes the most manga-ish part.
Create a new layer and set it to Normal. Don't clip it or it won't work.
Take the Brush Tool, adjust the size and draw a curvy white line following the inclination of the head.
Make it thick enough and as perfect as possible.
Now take the Water Tool and start blending the line. Try to leave a thin edge line in the upper part.
I am an idiot and I completely forgot it XD
If you forgot it too, you can draw a very thin line to fake the one we should have left in the upper part of our lighting.
Blend a bit where needed. Remember that we're aiming for a white light that gives a round-ish effect to the hair and makes it look better.
I think it looks better when you do it right and don't forget anything, anyway xD
Too much light doesn't look good too. That's why we're going to take the Eraser and erase some parts with a painting move.
If you do it right it won't look too rigid and turn out weird. Just do it like if you were using a normal brush and paint gently.
Song 2: Italy's Hatafutte Parade (TV size)
Optional: to give it a more colorful look we can add some colored lights.
To do so, choose a very bright color, take your pen, adjust the size (not too thin, not too big) and add some random strokes.
I suggest not to exaggerate. It'd look awful, trust me.
Finished