Austin arrived as Ukrainian President Volodymyr Zelensky urges his Western allies to lift restrictions on the use of long-range weapons and as he presses for an immediate invitation to join NATO.
"I'm pleased to announce today the commitment of a $400 million presidential drawdown package to provide your forces with additional munitions, armoured vehicles and anti-tank weapons," Austin said during a meeting with Zelensky.
The package was part of support previously announced by the White House for Ukraine.
In a later speech in Kyiv, he called for solidarity with Ukraine at a time when Kyiv fears the prospect of reduced US military support should Donald Trump be elected to the White House next month.
But he did not address Zelensky's call to join NATO or a "victory plan" the Ukrainian leader outlined last week that seeks enhanced Western support to defeat Moscow's troops.
"We face a hinge in history," Austin said.
"We can continue to stand firm against Putin's aggression. Or we can let Putin have his way, and we can condemn our children and grandchildren to live in a far bloodier and more dangerous world," he continued.
Austin's visit came a few days after South Korean intelligence said North Korea has sent thousands of soldiers to support Moscow's war in Ukraine.
Austin urged determination against "the spectre of an aggressive Russia, backed by other autocrats from North Korea to Iran."
About 1,500 North Korean soldiers are in Russia acclimatising and will likely head to the front lines, Seoul's spy agency has said, with more troops set to depart soon.
Ukraine is already facing tough battles, especially in the east where Russian troops have been making gains in the past few weeks.
As Austin was in Kyiv, Russia staged more aerial bombardments across the east and south of the country.
The governor of Zaporizhzhia region said at least three people were killed and a dozen more were wounded in a strike that damaged a kindergarten.
And at least six were killed in the eastern Donetsk region in several shelling attacks, regional governor Vadym Filashkin said on Telegram.
That figure included three killed in the key logistics hub of Pokrovsk, which is being heavily targeted by Russian forces under 10 kilometres (six miles) away.
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