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The Royal Navy is to help rescue those Britons stranded abroad by flight restrictions as the Transport Secretary tells Sky News Britain's airspace may open tomorrow.
With the UK no-fly zone being extended until 1am tomorrow, the Government says three ships could be used to help ferry travellers back home.
HMS Ocean will head to the Channel today and HMS Ark Royal will move "later" - with HMS Albion en route to Spain to pick up British soldiers.
Madrid may also be used as a hub for stranded tourists.
Mr Brown unveiled the measures after a meeting of the Government's emergency response Cobra committee called to deal with the fallout from Iceland's volcano.
HMS Ark Royal will be sent to rescue stranded Britons
"I talked to Prime Minister Zapatero and he has offered in principle use of Spanish airports as a hub to bring people back to Britain.
"And we are now looking if we can make the arrangements necessary, the transport arrangements that we will support as a government, coach, ferry and train to get people either from Madrid or another Spanish airport back to Britain," the Prime Minister said.
With pressure mounting to ease the flight restrictions, Mr Brown said passenger safety was "paramount".
Transport Secretary Lord Adonis said there was a chance Britain's airspace could open on Tuesday after a "dramatic decrease" in volcanic activity.
"It may be possible to start opening some UK airspace tomorrow," he said.
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Germany and Italy have extended flight restrictions until 6pm - Italy this morning briefly reopened its airspace in the north only to shut it a short time later.
Denmark said it was opening its airspace above 35,500ft while the Czech Republic said its airspace would be open for 48 hours.
The ash cloud is expected to hit the east coast of the US at 6pm.
Travel association Abta estimates around 150,000 Britons are stuck abroad.
Many of those on holiday over Easter were teachers and pressure is growing on the Government to get them back to the UK.
Liberal Democrat leader Nick Clegg, whose three sons are stranded in Spain, said he supported the Government's "wholly laudable" efforts to get people home.
Robert Nisbet Reports From Mount Eyjafjallajokull
First Choice and Thomson say they are launching rescue efforts to return 5,000 holidaymakers from the Spanish resorts of Alicante and Malaga, via train and ferries.
But pressure is mounting on European governments to ease the restrictions.
British Airways, which is losing up to £20m a day during the crisis, said a test flight yesterday suffered no damage and called for the blanket ban to be lifted.
However, glass build-up was found in an engine of a Nato F-16 fighter plane, a US official said.
The director-general of the airlines' trade body, the International Air Transport Association, described the European response as an "embarrassment" and said the flight ban was not based on "facts".
Giovanni Bisignani told the BBC Radio 4 Today programme: "This is a European embarrassment and it's a European mess. It took five days to organise a conference call with the ministers of transport.
"Europeans are still using a system that's based on a theoretical model, instead of taking a decision based on facts and risk assessment.
Met Office prediction of ash cover until Tuesday 0100 April 19
"This decision (to close airspace) has to be based on facts and supported by risk assessment. We need to replace this blanket approach with a practical approach."
Jim French, chief executive of Flybe, told Sky News the "blanket methodology" for the ban was incorrect and the Government would need to consider bailout packages for struggling airlines.
The IATA says the crisis is costing the industry £130m a day.
The fall-out from the travel crisis continues to be felt.
A toddler is in a life-threatening condition in hospital after her bone marrow transplant was delayed because of the flight ban.
The little girl, who cannot be named, was said to be in an "extremely vulnerable state" as restrictions remained.
They have prevented critical treatment arriving from a donor in Canada - her only hope of survival.
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