Roger Daltrey, who is an honorary patron of the Teenage Cancer Trust, said the rise in employers' national insurance payments could result in nurses being laid off.
The Who legend has played concerts to raise money for charity but suggested announcement last week will directly impact the services they can provide to some of the most vulnerable in society.
The changes in the Budget will mean charities will have to raise money to cover the increase in employers' NI contributions from 13.8 per cent to 15 per cent from April.
"If we can't raise more money, we will have to lay people off," he told The Daily Telegraph, saying he did not "like to think about the consequences" of getting rid of specialist nurses.
"To lose nurses would be catastrophic".
The level at which employers start paying the tax on each employee's salary will fall from £9,100 a year to £5,000
The National Council for Voluntary Organisations (NCVO) said the contributions will cost the charity sector, which employs around 3% of the UK workforce, around £1.4 billion annually.
"I'm incredibly angry because the Government is just throwing money at the NHS thinking that will solve all the problems, which it quite clearly won't, and it's being funded partly by taking money from charities like ours."
The 80-year-old singer, who was made a CBE in 2005 for his services to music and charities, said charities such as the Teenage Cancer Trust, Marie Curie Hospices and Macmillan Cancer Support nurses took "an awful lot of burden off the NHS" and the national insurance increase had "so little thought behind it".
Daltrey added that it was "really hard graft" to raise money for less well-known charities.
He explained that while private sector companies may be able to pass on the cost of extra NI payments to customers by raising prices, the same can't be said for charities, who have no option but to raise money at the cost of losing more staff, which is "heartbreaking".
NCVO chief executive Sarah Elliott said the planned national insurance increase would be "absolutely unsustainable" for many charities.
"Charities across the country are already in a dire situation, juggling a triple threat of rising demand, escalating costs and falling funding," she said.
"This additional cost, for which there is no headroom in budgets to cover, will be devastating."
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