"The whole aspect of this in terms of deciding that our safety and security depends on keeping people out rather than welcoming people and understanding what this country is about ... I think it's just flat anti-American," she told CNN's Chris Cuomo Tuesday on "New Day."
Albright, who endorsed Trump's presidential candidate opponent Hillary Clinton, said the idea that the ban will make America safer is a myth.
"I think this was the most unprepared plan that I have ever seen in terms of the lack of coordination with other parts of the government," she said. "It has actually created more danger because there are countries that are now, in fact, not able to cooperate with us in terms of intelligence sharing or generally mistrust, and there's going to be tit for tat."
Prior to Trump signing the executive order, Albright said she would "stand ready" to register as Muslim if Donald Trump takes executive action that affects immigrants traveling to the US.
"I was raised Catholic, became Episcopalian & found out later my family was Jewish. I stand ready to register as Muslim in #solidarity," she previously tweeted.
Trump is considering a ban on refugees for up to four months, according to a draft executive order. The move would make good on one of his most controversial campaign promises aimed at fighting terrorism. Trump has said the order enacting stronger measures on Muslim migrants trying to enter the US is a national security issue. In the days after his election, he also repeated his proposal of a national database to register all Muslims living in the US.
Albright was born in Prague in 1937 but eventually immigrated to the US to flee persecution from Nazis after stints in the UK and Czechoslovakia.
Albright, who endorsed Hillary Clinton in the 2016 election, also tweeted a photo of the Statue of Liberty with a quote: "Give me your tired, your poor, Your huddled masses yearning to breathe free, The wretched refuse of your teeming shore. Send these, the homeless, tempest-tossed to me. I lift my lamp beside the golden door," her photo said.
"America must remain open to people of all faiths & backgrounds," Albright added.
Albright is not the only high-profile public figure offering to register as a Muslim. Actress Mayim Bialik also tweeted in solidarity of the movement.
"I'm Jewish. I stand ready to register as a Muslim in #solidarity if it comes to that," she tweeted