The vote is likely to see the centre-left replace the ruling conservatives.
It could also see a new populist party, whose leader is on trial for alleged anti-Semitic comments, enter parliament for the first time.
Polling stations closed at 1700 GMT with a voter turnout of 52.06 percent and the results will likely be known overnight.
The Baltic state of 2.8 million people has been warily eyeing neighbouring Russia, fearing it could be the next target if Moscow succeeds in its war against Ukraine.
Lithuania's main parties all agree on the need for strong support for Ukraine and to maintain or increase defence spending, currently around three percent of GDP.
Opinion polls show the Social Democratic Party, which last led the government from 2012 to 2016, ahead of 14 other parties and coalitions. The latest survey suggested they would secure around 20 percent of the vote.
The ruling centre-right Homeland Union-Lithuanian Christian Democrats are expected to receive around 15 percent. Six or seven parties are likely to cross the electoral threshold required to win seats in parliament.
Despite the expected change in government, no major foreign policy changes are anticipated.
"There is no real alternative to what Lithuania chose 20 years ago," political analyst Linas Kontrimas told AFP, referring to the country joining the European Union and North Atlantic Treaty Organization.
- President's backing -
President Gitanas Nauseda, who won a second term in May with backing from the Social Democrats, is believed to support a change in government.
During the campaign, Nauseda -- who defeated Prime Minister Ingrida Simonyte in the presidential vote -- met with leaders of all parliamentary parties except the conservatives, whom he has frequently wrangled with.
"I voted for the authorities to work together, not against each other, to solve the problems of the Lithuanian people," Nauseda said after voting. He did not reveal his party preference.
"The time of the conservatives is over," Social Democratic leader Vilija Blinkeviciute, a former social security and labour minister, told reporters.
The Social Democrats have pledged to make taxation more progressive, tax luxury goods and provide additional funding for social services, as well as cut taxes for families with children, offer VAT relief on food and raise pensions.
- Anti-Semitism concern -
One 65-year-old pensioner, Julija, told AFP she could not live with her current allocation. "Everything is so expensive," she said.
But Monika, a 34-year-old lawyer, said she backed the government and voted for the status quo. "In recent years, Lithuania has developed despite the difficulties linked to the war," she said.
The election has been marred by controversy surrounding the populist Nemunas Dawn party led by former MP Remigijus Zemaitaitis, which is expected to win seats.
Last year, Zemaitaitis gave up his seat in parliament over alleged anti-Semitic comments. On trial for incitement to hatred, he denies the charge and insists he only criticised the Israeli government's policies in Gaza.
Most parties have vowed to exclude Zemaitaitis from any ruling coalition.
"I think we are facing not only a geopolitical threat, but also an internal political threat," Foreign Minister Gabrielius Landsbergis, leader of the conservatives, told reporters after voting.
During World War II, 90 percent of Lithuania's Jewish population of approximately 208,000 were killed, often with the help of local collaborators.
The first round of voting will allocate roughly half of the 141 parliamentary seats through proportional representation. The remaining seats will be decided in runoffs on October 27.
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