Tillerson was greeted frostily in the Russian capital as Lavrov began their meeting Wednesday by demanding to know America's "real intentions".
The United States and Russian Federation on Wednesday both presented souring views of the relationship between their two countries, exchanging sharp words as Moscow extended an icy welcome to the United States' top diplomat in a face-off over Syria.
Putin also said on Russian TV that the level of trust has "deteriorated". Beyond Syria, Russia's alleged meddling in the USA presidential election also hovered over what was the first face-to-face encounter between Putin and any Trump administration Cabinet member.
"We may be at an all-time low" in relations, Trump said at a news conference at the White House following a visit by the North Atlantic Treaty Organization's secretary-general.
Laying bare deep and risky divisions on Syria and other issues, President Donald Trump declared that USA relations with Russian Federation "may be at an all-time low".
The Moscow news conference came after Putin met Tillerson for the first time since Trump took office.
"We hope that the Russian government concludes that they have aligned themselves with an unreliable partner in Bashar al-Assad".
Only weeks ago it seemed Trump was poised for a potentially historic rapprochement with Russian Federation.
Russian Federation has vetoed another United Nations resolution against the Syrian regime in order to protect its ally Bashar al-Assad following the chemical attack in Idlib. "We'll see what happens".
But he said Moscow and Washington had agreed to continue co-operating to try to find a political solution for Syria.
Meanwhile, Mr Trump has also declared North Atlantic Treaty Organisation is "no longer obsolete" - and has said he is committed to the military alliance.
Lavrov, addressing a news conference, said that Moscow is ready to restore an air safety agreement covering Syria which it had suspended after last week's United States missile strikes on Syria.
"We have information that a similar provocation is being prepared... in other parts of Syria including in the southern Damascus suburbs where they are planning to again plant some substance and accuse the Syrian authorities of using chemical weapons", he said on Tuesday. "No", Trump said. But, he added, "I see them using gas. we have to do something". He said it was "unacceptable that the OPCW analyses the evidence not on location".
"I am absolutely certain that the USA supports this approach, partly because the United States is contributing with forces to our enhanced presence in the eastern part of the alliance, and also in the southeast of the alliance in Romania".
"Unfortunately, we've got some differences with regard to a majority of those issues", Lavrov lamented.