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I can connect to the PC via Remote app on the iPhone, but the iPhone can't see the PC to Sync and the PC won't recognize the iPhone. I've done syncing over WiFi before.

I'm using iPhone 3GS w/ iOS 6 and Windows 8.

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When you say you can connect via Remote, are you referring to the Remote App on the iPhone? – jbharper2 Dec 12 '12 at 5:31
Yes, I'm. I've also edited the question. – Peter Draex Dräxler Dec 12 '12 at 13:30

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Here are the standard steps to set it up:

  1. Make certain that your computer and iPhone, iPad, or iPod touch are connected to the same Wi-Fi signal.
  2. Connect your iPhone, iPad, or iPod touch to a Mac or PC via USB. Launch iTunes if it doesn’t do so automatically.
  3. Highlight your iDevice in the sidebar. (or choose at top right if iTunes11)
  4. Click "Summary" in the menu bar. Scroll down to the "Options" section.
  5. Check the "Sync with this (iOS device) over Wi-Fi" box. Click "Apply."
  6. Detach your iPhone, iPad, or iPod touch.
  7. Initiate an iTunes Wi-Fi Sync by tapping Settings > General > iTunes Wi-Fi Sync > Sync Now on your iPhone, iPad, or iPod touch. Or, plug it into an outlet

Does it fail at a particular point?

source

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I have the "Sync with this iPhone over Wi-Fi" option checked. After detaching the iPhone I can't initiate the sync. All I can see is "Sync will resume when DT2-NTB is available.". – Peter Draex Dräxler Dec 12 '12 at 13:39
@PeterDraexDräxler, in step 7 above, have you turned on the service on the phone itself? – JoshP Dec 12 '12 at 13:41
What service on the phone do you mean? I'm connected to a WiFi. – Peter Draex Dräxler Dec 12 '12 at 14:36
It's curious, now it works without changing any settings. This happens to me often. It sometimes works and sometimes does not. – Peter Draex Dräxler Dec 12 '12 at 14:37
@PeterDraexDräxler, hmmm, that is curious. That strikes me more as a network issue rather than an iTunes/iDevice issue. Does your Remote app ever fail to connect? – JoshP Dec 12 '12 at 14:40
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