More than 100,000 people would quit smoking in one year alone if the Chancellor increased the tax on cigarettes to 5% above inflation, according to 80 leading health charities and experts.
In a report released ahead of next week's Budget, campaigners are calling on Chancellor George Osborne to increase the tobacco "tax escalator" from 2% to 5% above inflation year on year.
The move would net the Government an extra £485 million in the first year and £7.4 billion over the next five years, it said.
Furthermore, it said the number of smokers would fall by 104,000 in the first year, with a reduction in deaths from smoking of 479.
A 15% rise above inflation for hand-rolled tobacco would lead to even more lives saved, far fewer smokers and further revenue, it added.
The report, from the charity Action on Smoking and Health (Ash) and the UK Centre for Tobacco and Alcohol Studies, is backed by NHS groups of doctors, directors of public health, the Royal College of Paediatrics and Child Health, and the Royal College of Physicians.
Charities including the British Heart Foundation (BHF), Cancer Research UK, and the Roy Castle Lung Cancer Foundation also back the study.
And it says there needs to be stronger support for new laws to introduce plain, standardised tobacco packaging, and asks for an update on the Government's anti-smuggling strategy.
It comes as a poll of more than 2,000 former smokers for the BHF found 42% believed raising the tax on tobacco would help other smokers quit.
Over two in five (43%) said GPs should approach the subject more often with smokers during routine appointments, while 35% called for more information about local stop-smoking services.
Nearly a third (30%) said reducing the number of smoking scenes in TV programmes and films would help people quit, while 34% wanted more information in gyms, offices and leisure centres.
Deborah Arnott, chief executive of Ash, said: "Raising the price of tobacco through taxation is the most effective way of reducing smoking and saving lives.
"Increasing taxes is a win-win for government - it raises much-needed revenue and encourages smokers to quit a deadly addiction. That is why we are calling on the Chancellor to be bold and raise the tax by 5% above inflation to further motivate smokers to quit."
Simon Gillespie, chief executive of the BHF, said: "This is not about nanny state intervention. This is about a practical measure that saves lives - and one that people who've managed to break their addiction to tobacco say will help.
"We know two-thirds of smokers want to quit and more than a million of them will try to do just that today - No Smoking Day.
"We hope their voice and their efforts will not go unnoticed by ministers, who also have 'big tobacco' whispering in their ear."
Anna Gilmore, professor of public health at the University of Bath and researcher at the UK Centre for Tobacco and Alcohol Studies, said: "Tobacco companies constantly complain about tax rises while at the same time quietly increasing prices and amassing huge profits from the sale of a product that kills half their long-term customers.
"This shows there is scope for raising tobacco tax. Increasing taxes not only helps smokers to quit but also deters children from starting a life-long addiction."