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Samsung reclaimed the spot from Taiwan Semiconductor, which made the chips for the last iPhone and iPad. Prior to that, Samsung had made the processors for all previous iPhones.
Last November, the Korea Times report that Samsung would replace Taiwan Semi, but not until 2016.
The win comes as Apple's iPhone sales continue to grow at the expense of Samsung's own high-end smartphones. Samsung's phone business also faces pressure on the low end from inexpensive Chinese Android phones.