While Romney and Bulger have been at odds for months, this was the first time the Republican governor had said that the UMass (search) president — a Democrat who led the state Senate for an unprecedented 17 years — was no longer fit to lead the state's flagship university system.
"I believe that the time has come for the president to place the interests of the students and the university above his own interests and step aside as president," Romney said. "I believe he should resign."
A day earlier, the state Senate rejected the governor's proposal to reorganize higher education and eliminate the UMass president's job.
Bulger's brother, James "Whitey" Bulger (search) is on the bureau's Ten Most Wanted list, sought in connection with 21 murders.
Bulger's spokesman said the UMass president "has no intention of leaving."
"The president was at work at the business of the university yesterday, he's at that business today, and he will be at that business for a long time to come," said spokesman John Hoey.
A congressional committee wants to question William Bulger about his brother's whereabouts and what contact he may have had with the fugitive since he fled in 1995, just before he was indicted.
When subpoenaed by the committee in December, the UMass president invoked the Fifth Amendment, refusing to answer any questions. He also appeared before a grand jury and later told reporters: "I don't feel an obligation to help everyone to catch him."
Democratic Attorney General Thomas Reilly became the first high-ranking state official to call for Bulger to step down earlier this week, arguing that the UMass president had chosen allegiance to a fugitive "mass murderer" over the interests of the university system.