Mr. Netanyahu said that the deal was “fatally flawed on weaponization,” referring to the military application of Iran’s enriched uranium, and that the documents proved it was based on a lie. He added that the cache of more than 100,000 pages was now being shared with the intelligence services of the countries that negotiated the agreement with Iran: the United States, Russia, China, France, Germany and Britain.

To those arguing that the documents did not prove any Iranian violation of the accord since it came into effect in 2016, Mr. Netanyahu said that was missing the point.

“If you don’t violate a dangerous deal, it doesn’t make it less dangerous,” he said, adding that the accord was based on “a fictitious Iranian report” to the International Atomic Energy Agency, in which Iran denied having ever planned to build a weapon.

Mr. Netanyahu also dismissed experts who said the documents just proved why a deal was necessary. “A deal that enables Iran to keep and hide all its nuclear weapons know-how is a horrible deal,” he said.

The accord gave Iran “unlimited enrichment in both ways,” he said, because it removed economic sanctions on Tehran and at the same time “gives them the ability to enrich uranium on an industrialized scale” when the restrictions in the deal end.

“The last thing you can say about it is that it blocks all of Iran’s paths to the bomb. In fact, it does the very opposite,” Mr. Netanyahu said. “If you do nothing to this deal, if you keep it as is, you will end up with Iran with a nuclear arsenal in a very short time.”

Mr. Netanyahu has staked his political career on blocking Iran and its nuclear ambitions, which pose a potential existential threat to Israel, but there is no sign so far that his campaign has shifted European leaders who have lobbied Mr. Trump not to scuttle the deal.