Benefits for those workers were scheduled to expire at midnight Tuesday night.
"It's unfortunate we cannot move this bill. We will try again," Sen. Jack Reed, D-R.I., said.
Opponents said the measure doesn't provide a way to finance the $56.4 billion in benefits. Sen. Scott Brown, R-Mass., accused Democrats of trying to pass the measure under last-minute pressure, and proposed using unspent or unobligated federal funds to pay for the benefits extension for long-term unemployed workers, The Hill reported.
Senate Republicans held up a benefits bill for nearly two months during the summer, the Capitol Hill publication said.
Sen. Max Baucus, D-Mont., said in a statement the legislation would reauthorize benefits for nearly 800,000 long-term unemployed who are about to exhaust their benefits next week, as well as extend benefits for 2 million more facing the same fate at the end of the year, CNN reported Tuesday.
Federal jobless payments, which last up to 73 weeks, take effect after state-funded 26 weeks of coverage expire. These federal benefits are divided into tiers, and the jobless person must apply to move into a new tier.
The House of Representatives already failed to pass a bill that would have given the unemployed workers another three months to file for the extended jobless benefits.
"Unemployment benefits are the only lifeline many workers in Montana and across the nation have left in this tough economy," Baucus said in his statement. "These benefits help millions of Americans put food on the table and roofs over their heads -- pumping money into our economy and helping to create jobs."
About 14.8 million Americans are unemployed, with about 6.2 million of them out of work for at least 27 weeks, CNN reported. About 8.5 million people are collecting unemployment insurance.