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My mom has an iPhone 5 with some exercise videos in the Videos app, which just total about 150MB.

After getting an iPhone 6S Plus, can those videos automatically transferred to the new iPhone through iCloud sync? I believe the new iPhone is set up as a new iPhone but not "restored from backup", and it may keep the new iPhone from having older stuff that isn't needed. But just the videos, can they be sync'ed by using iCloud?

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The right way to do this is to use iCloud Photos. All media in Videos.app on iOS should be either from the iTunes Store or synced from iTunes – non personal made videos should be in there.

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