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I think designing with mark-up can be helpful when doing design prototype. Designs / wireframes can be quickly tested with other team members. Static JPGs, on the other hand, relies on people’s imagination. However, I’m not so sure about it as a primary design tool.
Applying inner-shadows, glow effect, gradient, rounded-corners… are great visual effects. They can be easily applied using CSS3. However, I can imagine that when people design with markups, they would rely on these effects. They would look at their design and think “mmm… how to make the text pop? ah-ha, apply glow effect – it’s easy to do with CSS3!” This kind of thinking would produce very boring kitsch design. Any effect that’s complicated / illustrative / dimensional would not come to their mind because they cannot be immediately achieved using CSS3.
Yes, I know nothing is impossible with CSS3, but many complicated things are like puzzles, which are hard to solve and disruptive to creative flow. And it’s hard to chuck things out when it’s a complete engineering triumph but a design disaster.
But anyway, some people might be interested in this technique. Nevertheless, I wasn’t convinced by your article & example.