Graffiti including "Kill Israiel" (sic) was sprayed on buildings and footpaths in Woollahra, a Sydney suburb known for its Jewish community, in the early hours of Wednesday.
A car, believed to be stolen, which the perpetrators drove to the scene was set on fire.
Coming days after a Melbourne synagogue was firebombed and destroyed, Prime Minister Anthony Albanese likened a spate of anti-Semitic attacks to terrorism and said Australia had been diminished as a result.
In an emotional press conference at the Sydney Jewish Museum, the PM met Holocaust survivors and pleaded for calm among the community.
"The firebombed car when no one is there is aimed at creating fear, the graffiti is aimed at creating fear … it is cowardly and it is prejudiced," Mr Albanese said.
"They are acts which are aimed at promoting fear in the community and that by any definition, is what terrorism is about."
He pledged $8.5 million to upgrade the facility in the hope it would teach more Australians about the importance of consigning anti-Semitism to the past.
Anthony Albanese used a speech at the Sydney Jewish Museum to plead for calm. (Mick Tsikas/AAP PHOTOS)
NSW Police Commissioner Karen Webb said the Jewish community would be under stricter surveillance after the incidents, with resources increased.
That will include "high visibility" policing in densely populated Jewish neighbourhoods.
"We are taking police and dedicating them to the operation … so police will be out there, the community can expect to see officers that will come up and speak to people," she said.
Independent Wentworth MP Allegra Spender, who represents the federal electorate with the highest proportion of Jewish voters, said Jewish-Australians were "heartbroken".
"But when I talk to my broader community, and every Australian I've spoken to, they say 'that is not us, we do not tolerate this sort of behaviour'," she said.
Premier Chris Minns also condemned the attack, saying it was a hate crime.
"A violent act of destruction, clearly anti-Semitic, designed to strike fear into the community that lives in this part of Sydney," he told reporters.
The perpetrators, believed to be two males of slim build, aged between 15 and 20, wore face coverings and dark clothing.
Foreign Minister Penny Wong said acts of hate had no place in Australia and anti-Semitism was condemned wherever it occurred.
"Australian Jewish communities have a right to be and feel safe," she said on social media.
Holocaust survivors Ernie Friedlander, Mark Spigelman and Egon Sonnenchein met Anthony Albanese. (Mick Tsikas/AAP PHOTOS)
The Adass Israel Synagogue at Ripponlea in Melbourne's southeast was set alight in a pre-dawn attack on Friday.
Australian Federal Police have set up a special operation in response to the "likely" act of terrorism, which will investigate threats, violence and hatred towards the Jewish community and parliamentarians.
It will also investigate Wednesday's attack, the second recent incident in Woollahra after buildings and vehicles were targeted in November.
A ute was set on fire, and multiple cars, a restaurant and other buildings were graffitied with anti-Israel messages.
Two men are in custody, charged over that attack.
Executive Council of Australian Jewry co-chief executive Alex Ryvchin said it was designed to terrorise Jewish Australians.
"How long will this continue and with what horrors will it end?" he said.