The royal duo helped soldiers unload sandbags near their grandmother's residence at Windsor Castle since early morning.
Dressed in waterproofs and Wellington boots, the Duke of Cambridge and his sibling were filmed making an unannounced visit to the River Thames village of Datchet, west of London.
William, the 31-year-old second-in-line to succeed Queen Elizabeth II, left the military last year while Harry, 29, is still in the army.
The Queen has also provided feed and bedding to flood-hit Somerset farmers following UK's wettest January in 250 years.
On the princes' involvement in the relief effort, a Kensington Palace spokesman said: "They wanted to show their support for the flood victims and have joined the armed forces' relief effort."
Britain has been lashed by rain and wind since December. Hundreds of properties in the Thames Valley have been inundated after the river overflowed.
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