Had some fun speculating this morning. My picks so far:
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Instruct Surgeon General to reschedule marijuana. If he refuses, fire him and find someone who will.
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Withdraw all US military presence on foreign soil. Military equipment is to be handed over to the host country, with the exception of relatively bad actors (e.g. Israel), in such case it is handed to their opposition. The influx of soldiers will be converted into a military engineer force to repair and develop infrastructure nationwide, including affordable housing and public transit.
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Close Guantanamo bay, end the embargo on Cuba.
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Withdraw from NATO, halt all NATO funding.
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Halt all arms sales to foreign powers.
I'm keeping it to whatever I can do unilaterally, but go wild if you like. To (selectively) quote Flannery O'Connor, "You can do anything you can get away with, but nobody has ever gotten away with much."
[redacted] the nazis and make a cultural revolution to fully purge the racism out of the US.
Can't really think of anything particularly fancy nor specific at the moment.