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Pencil and paper, Illustrator, Photoshop, CSS/XHTML…each project and each designer is going to require a different combination of these tools to create mockups and prototypes. The tools you use will influence what you design, which is why I think it’s really important to start with pencil and paper…or whatever is the most free-flowing medium for you.
That said, having just sunk a couple of days of my life into learning what a heinous piece of crap Fireworks is for creating mockups (I could definitely have coded my ideas in that time) I am going to experiment with HTML/CSS mockups this year.
Thanks for the article!