The former first daughter announced Friday she would be leaving her role at the network to "continue focusing on my work at the Clinton Foundation and as Marc [Mezvinsky] and I look forward to welcoming our first child."
Clinton joined the network in December 2011, and in recent months, had come under fire for a reported $600,000 salary.
During her time at NBC, Clinton, 34, focused on "stories about remarkable people and organizations making a profound difference in our country and our world."
"We are thankful for all of Chelsea's contributions to NBC News over the past 3 years, said Alex Wallace, senior vice president of NBC News. "Chelsea's storytelling inspired people across the country and showcased the real power we have as individuals to make a difference in our communities. While she will be missed, we look forward to working with her in the future."
Clinton, who holds a Ph.D. in international relations from Oxford, hasn't ruled out eventually running for public office, and has taken on an expanded role at the Clinton Foundation. Her child with husband Mezvinsky is due sometime this fall.