Assyria started to decline in the the second half of the 7th century BCE. Ashurbanipal (r. 669-631 BCE) is considered the last great king of the Neo-Assyrian Empire.
After his death there were a number of power struggles, and the empire came to a screeching halt in 612 BCE. In that year, the Babylonians razed the capital Nineveh to the ground.
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The Assyrian Empire did not last long. They did concur several nations but by 670 BC, they were in major decline.