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Dundjinni is one I used to use.
I use Inkscape and Gimp now.
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Donjond20 generator has a ton of good stuff. NPC, treasure, encounters, magic shops, etc, and dungeons of various size, difficulty, and themes.
http://donjon.bin.sh/d20/dungeon/
I really like it and use it alot.
I started with Campaign Cartographer 2 then moved on to Dundjinni then to Photoshop/CC3.
Bar far the best bet is Photoshop with artwork from Dundjinni. In some cases I will use CC3 to start and then finish up in Photoshop.
Photoshop has a huge learning curve but it is so worth it.
Dundjinni is one I used to use.
I use Inkscape and Gimp now.
I would be careful about Dundjinni though. No one is minding the store, the original programmer has been in and out of contact over the last few years so It's a bit of a dodgy thing. I wish this wasn't the case because it really was a good program and much promise going forward.
Like Adamantine Dragon I've had to move on to other options. Currently I'm using a mix of vector drawing programs. TouchDraw and iDraw (both iPad), Artboard (Mac), even dabbled in using Sketchup. The big advantage of Sketchup is that it can be used render full 3D environments to scale and it's learning curve is actually fairly gentle for basic drafting. Make sure you grab the download under the Pro, there is a free version.