The 54-year-old actress starred in the role of Captain Victoria Gates since season four.
Jerald shared the news with her Twitter followers, revealing that she was "surprised and saddened" to hear that she would no longer be a part of the show, reported Deadline.
"To my Castle fans around the world," the update read. "As of late yesterday I am surprised and saddened to learn that I will no longer be a part of the Castle family. Thank you all for your support and love. Hugs from PJJ."
Nathan Fillion and Stana Katic will reprise their respective roles of Richard Castle and Kate Beckett.
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