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For us, the interface is a major selling point. It's simple and straightforward; you don't have to click through endless menus to get what you want. The browser-based interface on your computer is also handy, allowing you to thumb through your phone's entire photo stream. You can also have the photos open automatically in a photo app when sending them to your mobile device, though this isn't the first app to offer such functionality.
Photo Transfer App gets the job done, but it isn't perfect. One frustration in the browser interface is that the (virtual) buttons were at times simply unresponsive. We had to click three times in one case to download a batch of photos. Is this a deal breaker? Not really. But it is annoying.
One other annoyance (which might be a deal breaker) is that when selecting photos, Photo Transfer arranges your shots into groups with a maximum size of 100, rather than simply placing them in one large pool or grouping them in folders according to date. If you take a lot of shots, it can be difficult to locate the one you're looking for, which was our experience. Who knows off the top of their head that the shot of your cat you want was 563 photos ago?
Another sticking point for some smartphone shutterbugs could be that the app doesn't automatically sync the photos for you, so you'll have to actively be working on both your desktop and/or mobile device. If that's your case, iCloud is a much better option.
If you have specific photos you want to sync between lots of different devices, this could be more convenient than syncing though the cloud. However, the grouping of your photos by hundreds makes us want to find another photo transfer app for our personal use.