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Yes you could do that!
The pictures taken from the phone camera are ''distorted'' by the lenses and the focal of your camera. You definitively could take picture/video directly from your phone and calibrate with a PC tool. I think this is the best way to do this.
If you need to calibrate any phone device directly with your application, it will be very slow! Consider taken pictures (possibly with the android build-in camera application) and perform calibration with a native call to OpenCV but offline due to the time requested by such computation.
