The exit poll gave the Kukuriku coalition led by the Social Democrats (SDP) 44.5 percent of the vote against 22.1 percent for the ruling conservative Croatian Democratic Union (HDZ), national television HRT reported.
If confirmed, the results translate into 82 seats in the 151-seat parliament for Kukuriku against 40 seats for the HDZ and its regional partners.
Partial official results based on between 10 and 20 percent of votes counted nationwide reflected the trend with the coalition projected to win 78 seats against 48 for the HDZ.
The electoral commission is releasing percentages for each constituency while the national television translates them into seats.
OUT OF CRISIS
Croatia's new government will face the difficult task of steering the Balkan country's economy out of crisis and taking it into the European Union in July 2013.
Vesna Pusic, an official with the coalition's junior HNS party who is also likely to be foreign minister, vowed the bloc would live up to voters' expectations.
"We really take that seriously and we will work hard... It gives us a strong mandate and a big obligation," she told national television.
SDP leader Zoran Milanovic had voiced confidence over the outcome as he cast his ballot in Zagreb, telling reporters: "We expect victory".
"I hope the citizens will have confidence in us. The central issue in these elections, as we have been saying all the time, is confidence," the 45-year-old former diplomat said.
Dina Vrdoljak, a 22-year-old law student, said she voted for Kukuriku "because we have such an unbelievably high level of corruption," echoing the outrage of many over a string of corruption scandals involving the HDZ.
"I do have hope and I expect a change," she said.
SLOW GROWTH
Croatia became independent in 1991 but was ravaged by war until 1995. Its economy then boomed notably thanks to Adriatic tourism but growth came to a brutal halt with the 2008 global financial crisis.
With growth now crawling at 0.5 percent this year and unemployment soaring to 17 percent, the new government will have to create jobs, reform the welfare system, cut down red tape and avert a credit rating downgrade.
"We are not sure what awaits us. Sweat definitely -- but I believe without blood and tears -- and a lot of uncertainty," Milanovic said ahead of the exit polls, pledging to lead the country in a "more honest and efficient way".
The remarks were a swipe at the HDZ which has been in power almost continuously since the 1991 break-up of the former Yugoslavia, with surveys showing that Croatia's electorate still has little trust in its politicians.
HDZ leader and current Prime Minister Jadranka Kosor launched an anti-graft drive, a key EU demand, when she was appointed in 2009 but it backfired.
Kosor's powerful HDZ predecessor Ivo Sanader is on trial for corruption while the party is being investigated over alleged use of slush funds.
More than 4.5 million Croatians were eligible to vote. Three hours before polling stations closed, turnout was at 46.06 percent, about two percent lower than the last elections four years ago, the electoral commission said.
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