Ministers blamed the increase on a switch from gas to coal for electricity generation, but environmental groups said Britain was making no real progress on cutting emissions.
The UK produced total greenhouse gas emissions equivalent to 658.1 million tonnes of last year. This was down about 15 per cent from the 1990 figure of 775.2 million tonnes.
But output rose from 544.2 million tonnes in 2005 to 560.6 million tonnes in 2006, a significant rise compared with previous years.
Tony Juniper, the director of Friends of the Earth, said: "These pathetic figures highlight the need for tougher action to tackle climate change.
"Government proposals for a new climate-change law must include annual targets for cutting carbon dioxide emissions by at least 3 per cent each year. This would force successive governments to put climate change at the core of all their policies and ensure that the UK moves towards a low-carbon economy.
"Most of the solutions to climate change already exist. It is the political will that's lacking."
Charlie Kronick, of Greenpeace, said: "2006 was the year of government green spin, but the numbers don't lie. For all the announcements and new reports, only one thing really matters - is New Labour reducing Britain's carbon footprint? And the answer is no."
Yesterday's figures do not include emissions from the UK's share of international aviation and shipping, which are rising even faster.
Between 2004 and 2005, emissions from international aviation rose 5.7 per cent due to a greater number of flights. Between 1990 and 2005, emissions from aviation fuel use more than doubled.
A public consultation on what the government's new climate law should contain ends in June.
David Miliband, the Environment Secretary, said yesterday: "Any increase in carbon dioxide emissions is worrying, even though these figures do not include the effect of emissions trading.
"While these figures are provisional, they underline why concerted effort to tackle climate change, both from government and wider society, is absolutely critical. The Climate Change Bill is a central part of that drive. It will set the long-term legal framework for reducing emissions over the next 45 years and beyond, helping to enable the transition to a low carbon economy and provide a foundation for galvanising international resolve.
"Despite this year's provisional figures, we have a good foundation to build on. We're still on track to almost double our Kyoto commitment, with an estimated 23.6 per cent reduction in greenhouse gas emissions on 1990 levels by 2010, and we expect the long-term downward trend to continue."
He said the projected increase for last year demonstrated the effect external forces, such as fluctuating fossil fuel prices, could have on annual emissions.
While he acknowledged the need for decisive action, Mr Miliband said there was evidence of a real shift in attitudes.
"In 2005, household carbon dioxide emissions decreased 4.6 per cent on the previous year and I'm hopeful that, when the final 2006 figures are available, there may be evidence of a continuing trend as more people make changes to their everyday lives," he said.
Peter Ainsworth, the shadow environment secretary, said: "Only last Monday, David Miliband was boasting about how well the government is doing on cutting carbon emissions. But these figures prove that, contrary to what he has said, we are still heading in the wrong direction and have nothing to boast about.
"For all the spin and rhetoric, Labour is failing on climate change."