The "30 Rock" star was riding his bike the wrong way at 16th Street and Fifth Avenue near Union Square Park in Manhattan when he was stopped at about 10:15 a.m. and asked to show identification, they said.
That's when Baldwin, 56, refused to show his ID and acted belligerently, prompting the officers to handcuff him and take him, and his bicycle, to a nearby precinct, they said.
Baldwin was issued two summonses - for riding a bike the wrong way down a street and for disorderly conduct - and was then released, police said.
He is scheduled to appear in Manhattan Criminal Court on the disorderly conduct summons July 24.
A representative for Baldwin didn't immediately return a request for comment. But from his verified Twitter account, Baldwin said he'd been handcuffed for riding the wrong way on Fifth Avenue and posted the last name and badge number of the arresting officer.
He also tweeted that photographers outside his home terrified his daughter and disparaged New York City, calling it "a mismanaged carnival of stupidity."
The Oscar- and Tony-nominated-actor is known for his incendiary temper, most notably exposed when a voice mail of him berating his now-teenage daughter, Ireland Baldwin, came to light in 2007. He later said the message horrified him.
He was kicked off a plane in 2011 after refusing to stop playing a cellphone game, and he's gotten into confrontations with news photographers.
His personal life also was splashed into public last fall when he and his wife testified against a Canadian actress accused of stalking him. The actress, Genevieve Sabourin, was convicted after a Manhattan trial that delved into what she said was a steamy date and years of the actor stringing her along romantically. He said it was simply a professional dinner that degenerated into her harassing him.
In February, Baldwin wrote a New York magazine cover story decrying the constant tabloid coverage of his comings-and-goings in New York City, saying he "probably" needs to move out of the city and suggested he may soon be calling Los Angeles home.