Starmer announced the GBP21.7 billion investment over 25 years to support three carbon capture projects in Teesside and Merseyside in northern England.
"It is a landmark week in our national story, because this week we saw the end of coal, the power that built this country for many years," Starmer said, speaking in Chester, near Liverpool.
"Now... we see the new future on our horizon with carbon capture and storage, the largest programme in this new and vital industry anywhere in the world."
Britain's last coal-fired power station closed at the start of the week, boosting the country's ambitions to become carbon neutral by 2050.
The new investment will help fund "two carbon capture clusters" in the regions which have suffered from industrial decline.
The government says it will attract another GBP8 billion in private investment.
Speaking at a glass factory, Starmer admitted the need for cleaner energy to meet UK climate goals while hoping the mitigate some of the pains accompanying energy transition.
"Decarbonisation does not mean deindustrialisation," he said, assuring that "the timing is right" for the technology.
- Job creation -
The new Labour government has launched a flagship public-owned body, Great British Energy, to spur investment in renewable projects to meet net zero targets.
It hopes the carbon capture projects will create 4,000 jobs and support another 50,000 in the long term while removing 8.5 million tonnes of carbon emissions each year.
Carbon capture, utilisation and storage (CCUS) is a technology that seeks to prevent emissions created by burning fuels for energy and from industrial processes from releasing into the atmosphere.
The carbon is captured and then stored permanently in various underground environments.
According to Starmer, the UK continental shelf holds "a third of exploitable carbon storage space in all of Europe".
The investment will also help fund transport and storage networks to move the carbon to geological storage in Liverpool Bay and the North Sea.
While the technology has been discussed in government for over a decade, the latest announcement will see the first carbon dioxide stored from 2028.
F - 'Global race' -
The previous Conservative government had committed around GBP20 billion to be spent over 20 years on CCUS, however Starmer claimed that the Tories had not finalised any agreements or set money aside.
Accusing previous administrations of being "too slow" on the matter, Starmer reaffirmed that "carbon capture is a race that we can win".
Citing similar moves across Europe and the United States, Starmer said developing carbon capture technology was a "global race".
"This is a race, a global race... I am really pleased that we're putting ourselves in a position not just to be in that global race, but to win", he said.
Independent government advisers the Climate Change Committee welcomed the move as "very reassuring" on Thursday. The International Energy Agency considers the technology "critical" to achieving net zero.
However, environmental activists like Greenpeace UK criticised the plans as threatening to "extend the life of planet-heating oil and gas production."
Last month, UK climate scientists wrote a letter to Energy Security Secretary Ed Miliband arguing that CCUS relies on "unproven technology".
The letter warned that the plan would "lock the UK into using fossil fuel based energy generation to well past 2050".
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