The US and Iran clashed on security and human rights on Wednesday, with Iran's president demanding US guarantees to revive the 2015 Iran nuclear deal and the US president vowing Tehran would never get an atomic bomb.
Raisi said Tehran wanted former US President Donald Trump to face trial for the 2020 killing of Iran's top Quds Force commander Qassem Soleimani in a US drone attack in Iraq, holding up a picture of the general.
"There is a great and serious will to resolve all issues to revive the (2015 nuclear) deal," Raisi told the UN General Assembly. "We only wish one thing: observance of commitments."
Speaking later, US President Joe Biden reiterated his willingness to revive the nuclear pact under which Iran had agreed to restrain its atomic program in return for relief from economic sanctions.
In 2018, Trump withdrew the United States from the nuclear deal and unilaterally reimposed sanctions that have hobbled Iran's economy.
A year later, Tehran reacted by gradually violating the deal's nuclear limits and reviving international fears that Iran may be seeking to obtain an atomic weapon.
Raisi also sought to deflect criticism of last week's death of 22-year-old Mahsa Amini, who was arrested by morality police in Tehran for "unsuitable attire". Amini's death has unleashed anger in the streets since Friday over issues including freedoms in Tehran and an economy reeling from sanctions.
At least seven people have been killed in protests with some demanding "regime change".
Biden expressed a willingness to return to the nuclear deal, formally known as the Joint Comprehensive Plan of Action, and made clear US sympathies lay with the protesters in Iran.
"While the United States is prepared for a mutual return to the Joint Comprehensive Plan of Action if Iran steps up to its obligations, the United States is clear: We will not allow Iran to acquire a nuclear weapon," he said, repeating a long-held US position.
"We stand with the brave citizens and the brave women of Iran who right now are demonstrating to secure their basic rights," Biden added.