In a phone call with US Secretary of State Antony Blinken, Bennett called instead for "concrete measures" to be taken against Iran.
Bennett has been a consistent opponent of the 2015 agreement the powers have been seeking to revive.
He said "Iran was carrying out 'nuclear blackmail' as a negotiation tactic and that this must be met with an immediate cessation of negotiations and by concrete steps taken by the major powers," a statement from his office said.
It said Blinken had updated Bennett on what had been happening in the talks since their resumption on Monday after a five-month hiatus.
The Israeli leader expressed concern about a new report from the UN nuclear watchdog issued during the talks which he said showed Iran had "started the process of enriching uranium to the level of 20 percent purity with advanced centrifuges at its Fordo underground facility".
A year after then US president Donald Trump pulled out of the nuclear agreement in 2018 and started imposing sweeping sanctions, Iran began a gradual suspension of its undertakings in the deal.
The countermeasures have seen Iran enrich uranium in greater quantities and to higher levels of purity than it had agreed, something Western governments are eager to end as quickly as possible.
In April Iran said it would start enriching uranium up to 60 percent after an attack on its Natanz plant which it blamed on Israel.
The chief of Israel's Mossad external intelligence agency, David Barnea, said Thursday at an internal ceremony in Jerusalem that a "bad" Iran deal was "intolerable."
"It's clear there is no need for uranium to be enriched to 60 percent for civilian purposes. There is no need for three enrichment sites and there is no need for thousands of active centrifuges unless there is an intention to develop a nuclear weapon," Barnea said.
"A bad deal, which I hope they do not reach, is intolerable from our perspective."
Blinken, commenting in Stockholm after his call with Bennett, said Iran can't "sustain the status quo of building their nuclear programme while dragging their feet on talks. That... will not happen."
Iran insists the absolute priority is the lifting of all US sanctions imposed after Trump's abandonment of the deal.
The remaining parties to the 2015 agreement -- Britain, China, France, Germany and Russia -- have been participating directly in the Vienna talks. At Iran's insistence, the United States is doing so only indirectly.