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So complicated question! Heart and Brain both are most important organs of a alive body. Damage of any of them can result into sudden death.
Now, which does kill faster? It depends, which part of Brain/Heart is damaged. But if the sensitive parts of both are damaged then Brain will kill fast as it can survive only 6-8 second without Oxygen supplement, on other side even a heart transplant is possible.
So, Brain kills faster than Heart when shot .