"Ukrainians are making progress, are making advances," he said in the Oval Office.
Stoltenberg, visiting ahead of July's NATO summit in the Lithuanian capital Vilnius, gave insight into how the powerful Western military bloc sees Ukraine's attempt to turn the tables on Russia.
Ukrainians have talked optimistically about their long-prepared counter-attack across fronts in the east and south eventually driving Russian troops from the entire country.
Stoltenberg emphasized the operation as a way to gain negotiating leverage.
"The more land the Ukrainians are able to liberate, the stronger hand they will have at the negotiating table," he said.
Biden welcomed Stoltenberg, who is due to step down at the end of his term in October, saying that NATO's reaction to the Russian invasion of Ukraine had made the alliance stronger.
"We've strengthened NATO's eastern flank, made it clear we'll defend every inch of NATO territory. I say it again: the commitment of the United State to NATO's Article V is rock solid," Biden said, referring to the pledge by members to come to each other's defense.
"At our summit in Lithuania next month, we're going to be building on that momentum," Biden said.
Earlier, Stoltenberg told CNN that it was "still early days" for the offensive, which he characterized as "difficult."
Meanwhile, the US State Department announced a new $325 million package of ammunition and heavy weaponry to top up Ukraine's supplies as its big attack gets underway.
The Pentagon said the package provides "key capabilities to aid Ukraine's efforts to retake its sovereign territory and support Ukraine's air defenders as they bravely protect Ukraine's soldiers, civilians, and critical infrastructure."
- China warning -
Russian President Vladimir Putin ordered an invasion of neighboring Ukraine in February 2022, quickly seizing large areas of territory, but meeting fierce -- and growing -- resistance.
Stoltenberg said Ukrainians "have the right... to liberate their own land."
But he also characterized the Western decision to back Ukraine as part of a broader strategy to maintain stability around the world.
"Russia's brutal invasion of Ukraine was not only an attack on Ukraine, but also on our core values, and on free people everywhere. And therefore, President Putin must not win this war because that will not only be a tragedy for Ukrainians, but it will also make the world more dangerous," he said.
"It will send a message to authoritarian leaders all over the world, also in China, that when they use military force, they get what they want."
The NATO chief's meeting with Biden was scheduled for Monday but postponed after the US president had to undergo dental work.
Referring to the politics around who will replace him after his term as NATO chief ends, Stoltenberg told CNN: "I'm absolutely confident that they will find an excellent successor. My focus now is to lead this alliance until my tenure ends, because we are in the middle of a war in Europe."
"We believe the secretary general has done a fantastic job," Press Secretary Karine Jean-Pierre said when asked if Biden would ask Stoltenberg to stay on longer in the job, while stressing the president "hasn't made any decision yet" on whom he'll support to take on the role.
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