The White House says the decision was taken because those entities "no longer serve American interests".
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Nearly half of the 66 affected bodies are UN-related, including the Framework Convention on Climate Change - a treaty that underpins all international efforts to combat global warming.
Groups working on development, gender equality and conflict - areas the Trump administration had repeatedly dismissed as advancing "globalist" or "woke" agendas - are also included.
The White House said the decision was taken because those entities "no longer serve American interests" and promote "ineffective or hostile agendas".
The memorandum was signed on Wednesday after a review into causes that the White House said were "a waste of taxpayer dollars".
"These withdrawals will end American taxpayer funding and involvement in entities that advance globalist agendas over US priorities," it said in a statement.
It added that many of the organisations promoted "radical climate policies, global governance and ideological programs that conflict with US sovereignty and economic strength".
As well as the UN Framework Convention on Climate Change, the US has also withdrawn from the Intergovernmental Panel on Climate Change (IPCC) - the world's leading authority on climate science.
Non-UN organisations affected include those focused on clean energy cooperation, democratic governance and international security, such as the International Solar Alliance, the International Institute for Democracy and Electoral Assistance and the Global Counter-Terrorism Forum.
Trump has already stripped many multilateral organisations he dislikes of funds and previously rejected the scientific consensus of man-made climate change as a "hoax".
While the US Constitution allows presidents to join treaties "provided two thirds of Senators present concur", it does not specify what happens if they were to withdraw, which means Trump's move could face legal challenges.
These latest withdrawal