During the discussion, which has been described by the White House as "very good", the presidents agreed that the conflict in Syria has gone on "far too long".
The two evidently agreed to continue chatting by phone, but also spoke of having a personal meeting around the G20 summit in Hamburg, Germany (to the disappointment of whomever was pinning hopes on those Russian reports that their first face to face meeting would take place in May).
Despite Trump's entreaties to Putin during the presidential campaign, Syria has remained a source of tension.
The two leaders "spoke about how best to resolve the very risky situation in North Korea", according to a White House statement, which provided no further details on how they will respond to a series of nuclear detonations and missile tests conducted by North Korea's military. The U.S. action was accompanied by a dramatic shift in the Trump administration's rhetoric toward Russian Federation, one of the Syrian government's most important benefactors.
But following the April news that Assad - whose regime is propped up in part by Russian Federation - had gassed his own people, many of them women and children, Trump made the extraordinary decision to bomb Syria, provoking a harsh reaction from the Kremlin.
U.S. President Donald Trump speaks at an event with the Independent Community Bankers Association in the Kennedy Garden of the White House May 1, 2017 in Washington, DC.
Mr Trump's latest positive overtures towards Russian Federation come amid ongoing controversy over alleged collusion between his election campaign team and the Kremlin. The two leaders also discussed terrorism in the Middle East more broadly and the dangers of the North Korean nuclear program, the White House said.
The United States would send a representative to the cease-fire talks in Astana, Kazakhstan on May 3-4, the statement added.
Trump and Putin also talked about Syria, although the issue of an alleged chemical weapons attack by the Damascus government which was used to justify the cruise missile strike was not touched upon.
Sky's US Correspondent Amanda Walker said: "Donald Trump's admiration for Putin during the election was baffling". "If Russia has the influence in Syria that it claims to have, we need to see them use it".
The call came on the same day that Trump's 2016 campaign foe, Hillary Clinton, gave her most extensive interview since the election and blamed Putin, in large part, for her loss.
During his January call with the Kremlin, Trump was joined in the Oval Office by Vice President Mike Pence, chief of staff Reince Priebus, then-National Security Adviser Michael Flynn, chief strategist Steve Bannon and press secretary Sean Spicer.
Trump's effort to ease tensions coincided with a visit to Russian Federation by Chancellor Angela Merkel of Germany, who met with Putin in the southern resort city of Sochi.