The new Zune browser is surprisingly good, but not as good as the iPod's. It works well, but isn't as fast as Safari, and has a clunkier interface. If you occasionally plan on using the web browser that's not an issue, but if you're planning to browse the web alot from your PMP then the iPod's larger screen and better browser may be important.
If you're still on the fence: grab your favorite earphones, head down to a Best Buy and ask to plug them into a Zune then an iPod and see which one sounds better to you, and which interface makes you smile more. Then you'll know which is right for you.
Zune and iPod: Most people compare the Zune to the Touch, but after seeing how slim and surprisingly small and light it is, I consider it to be a rather unique hybrid that combines qualities of both the Touch and the Nano. It's very colorful and lovely OLED screen is slightly smaller than the touch screen, but the player itself feels quite a bit smaller and lighter. It weighs about 2/3 as much, and is noticeably smaller in width and height, while being just a hair thicker.