Tillerson accused Iran of intensifying multiple conflicts including the one in Syria, undermining U.S. interests in several countries, continuing to support attacks against Israel, and sponsoring cyber and terror attacks across the world.
However, addressing reporters in Washington, Tillerson branded the deal a failure, adding that Trump had ordered a review to evaluate whether the lifting of sanctions was "vital to the national security interests of the United States".
The secretary of state then specifically addressed the Obama administration's nuclear deal with Iran.
He said it delayed rather than blocked Iran's goal of becoming a nuclear state, ignoring arguments even by critics that it has reduced a significant security threat for now.
The state department is obliged to inform Congress every 90 days about Iran's compliance with the deal.
Iran denies ever having considered developing atomic weapons although nuclear experts have warned that any USA violation of the nuclear deal would allow Iran also to pull back from its commitments to curb nuclear development.
Tillerson is also likening Iran's behavior to that of North Korea.
In the deal, countries were to lift trade sanctions against Iran, in exchange for the country halting development on its nuclear programme.
Aside from the nuclear deal, Trump accused Iran of destabilizing the Middle East and wreaking havoc in Yemen, Iraq and Syria.
During last year's presidential campaign, he called for dismantling or renegotiating it. "It is another example of buying off a power who has nuclear ambitions and we buy them off for a short period of time and someone has to deal with it later".
"It would more isolate the United States than it would isolate Iran", he said, noting that other world powers are party to the deal.
At a ceremony in the Oval Office surrounded by steel executives, Mr Trump said it was a "historic day for American steel", saying his administration would "fight for American workers and American-made steel". White House press secretary described the attention as a sign that Trump believes there are problems with the deal. With some of those critics now in office, Tillerson's comments Wednesday marked the first time that position has been echoed by the USA government. On the one hand, Trump wants to show he's being tougher than Obama toward Iran, but on the other hand, he's not yet ready to rip up the deal.
Left unchecked, Middle East nation can "travel the same path as North Korea", Tillerson says.
Trump has followed through with a pledge to pull the US out of the Trans-Pacific Partnership, a sweeping free trade deal president Barack Obama negotiated.