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No but they do seem to have a very close relationship, like brother when leaving a sister (Ichimaru leaving Matsumoto). It seems that Ichimaru Gin would not hesitate to destroy anyone who wants to kill him except Matsumoto. It is seen that Ichimaru gave food to Matsumoto when she was the verge of dying of hunger. Therefore in the manga it was shown Rangiku was running toward Gin to stop him.

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