The two men held five hours of discussions at a German government villa on Wednesday before breaking off late in the evening.
As they began their talks Iranian President Mahmoud Ahmadinejad issued a defiant message that Iran would "not back down" on its nuclear rights in the face of pressure from Western powers.
"They want to use suspension (of nuclear enrichment) for propaganda and tell the world that they forced Iran into accepting suspension," Mr Ahmadinejad was quoted as saying by the official IRNA news agency.
"They are making a mistake and the Iranian nation will not back down on its rights."
Last ditch efforts
European diplomats have portrayed the talks as a last opportunity for Iran to agree to UN Security Council demands to suspend uranium enrichment activities and thus avoid the threat of UN sanctions.
The deal offered by the five permanent Security Council members plus Germany calls on Iran to accept a package of incentives in exchange for it halting enrichment.
The West fears that enriched uranium could be used to produce nuclear arms, although Iran rejects claims it’s trying to develop such weapons.
Key to the success of the talks is the question of whether Iran is prepared to suspend uranium enrichment for a limited period of time before or even during full negotiations with world powers.
The Washington Times reported on Tuesday that Iran was close to agreeing a secret deal that would see it suspend enrichment for 90 days while talks take place with European nations.
But Mohammad Saeedi, the deputy head of Iran's atomic agency, denied the reports.
"Since no negotiations have started this news cannot be correct and it is utterly baseless and without foundation," Mr Saeedi told AFP by telephone from Berlin before the meeting.
European diplomats said Mr Larijani made an offer at his last talks with Mr Solana on September 9-10 in Vienna, but several Iranian officials have denied any suspension is on the cards.
The US State Department said signs were "hopeful" signs from Iran but warned that sanctions were still on tap if diplomacy failed.
Iran insists its nuclear program is solely for energy needs and vehemently rejects US allegations that it is seeking to manufacture nuclear weapons.
According to European diplomats, Western powers have set the start of October as a final deadline for Iran to give its definitive response to the Security Council offer.