The United States and the Soviet Union signed the Intermediate-range Nuclear Forces Treaty (INF) in 1987, during the tail end of Ronald Reagan's presidency.
Mr Pompeo said the choice was to "bury our head in the sand" or "take common sense action" - arguing that the U.S. would "welcome a Russian change of heart" but had not seen evidence suggesting it is likely to comply.
Pompeo said there was no reason why the USA "should continue to cede this crucial military advantage" to rival powers. "It is now up to Russian Federation to preserve the INF treaty".
The U.S. has shared intelligence evidence with its North Atlantic Treaty Organisation allies that Russia's new SSC-8 ground-fired cruise missile could give Moscow the ability to launch a nuclear strike in Europe with little or no notice.
Although NATO Secretary-General Jens Stoltenberg said there would now be an intense diplomatic push to try to convince Russian Federation to give up what Pompeo said were "multiple battalions of the SSC-8 missiles", Washington is set to pull out of the treaty in February.
If Russia does not comply within the 60-day deadline, the USA will begin the six-month process of formally withdrawing from the INF treaty.
"It makes no sense for the United States to remain in a treaty that constrains our ability to respond to Russia's violation", Pompeo said, adding that: "The United States today declares Russian Federation in material breach of the treaty and we will suspend our obligations unless Russian Federation returns to full and verifiable compliance".
China, North Korea, and Iran are not obligated by the treaty's limitations, and, "This leaves them free to build all the intermediate range missiles they would like", he said.
Daryl Kimball, executive director of the Arms Control Association, warned that failing to negotiate a solution with Moscow "risks the start of a new missile race in Europe that will undermine European security". "We hope that they'll change course, but there's been absolutely no indication that they'll do so".
"We need to create a coordinated response to the actions of Russia", Klimkin said, adding that he raised "a set of practical steps with a number of proposals" at the meeting as to how NATO, Ukraine and Georgia might do that together.
There was no immediate response in Moscow to Pompeo's announcement, but Russian Defense Minister Sergey Shoygu said earlier on Tuesday that he and President Vladimir Putin had discussed how to take measures to increase Russian troops' "military capabilities" in response to a potential new "arms race".