Mr. Carey, 81, died Monday at a West Palm Beach, Fla., hospital. But he left a legacy here.
Mr. Carey died of heart disease Monday morning, surrounded by family members who had flown across the country to be at his bedside.
"He was just a remarkable talent and a visionary, and a generous man," said Gov. Martin O'Malley.
Mr. Carey had a lifelong passion for education because he thought that it would help the U.S. become more competitive in the global economy, so it's not surprising that the two largest beneficiaries of his philanthropy locally were Maryland universities.
In April, he donated $30 million to the University of Maryland School of Law, the largest gift in the institution's history. The philanthropist also made a $50 million bequest in 2006 to found the Johns Hopkins University's Carey School of Business, and in 2003, he gave $10 million to Gilman School.
Governor O'Malley described Mr. Carey as "a good friend" and campaign contributor, and said the men last saw one another two months ago.
"He was a person who understood that the world of business, the world of education, the world of art and the world of politics are not separate worlds. They are very much connected and need each other," he said.
Other Baltimore schools also were the recipients of Mr. Carey's generosity, including the Baltimore School for the Arts, the Bryn Mawr School and Calvert School. In addition, he gave $50 million to Arizona State University for that institution's business school, which is named for him.
"I don't have words to say how saddened I am that he has died," said Phoebe Haddon, dean of the University of Maryland's Francis King Carey School of Law, named for Mr. Carey's grandfather.
"Even though he'd lived in New York for six decades, he really felt that Baltimore was his home. He was so in love with the idea of re-creating the past grandeur that Baltimore had when his grandfather was alive. His strategy was to strengthen institutions like the University of Maryland law school."
Mr. Carey was a direct descendant of former James K. Polk, the 11th president of the United States, and had commissioned gold $1 coins that were engraved with the likeness of his illustrious ancestor.
"Those coins were in his pocket at all times," Dean Haddon said. "If he met you and liked you, he'd pull one out and give it to you, and tell you a little bit about his history."
Other friends received copies of a booklet of lithographs that Mr. Carey had commissioned of paintings of key moments in Baltimore's history, including the Great Baltimore Fire of 1904 and the founding of the first African-American church.
"He had a tremendous vision of what it means to be a good citizen," Dean Haddon said.
In fact, Mr. Carey never tired of speaking of James Carey, his great-great-grandfather, former chairman of the Bank of Maryland and a relative of Johns Hopkins. He reminded listeners that his grandmother, Anne Galbraith Carey, had created the Gilman School for Boys in Roland Park in 1897.
Former Baltimore Mayor Kurt L. Schmoke said Monday that he spent an interesting few hours chatting with Mr. Carey at the Orioles' opening-day game on April 4.
"He told me about all the connections of family members with Johns Hopkins and with the University of Maryland and with the city, and he seemed very proud of those connections. So it didn't surprise me when I learned of his contribution to the University of Maryland law school," Mr. Schmoke said. "I had a delightful time talking baseball and Maryland history with him."