The head of the Open University, who received a salary of more than £300,000, was Britain's best-paid academic last year, according to a survey of 164 universities.
University heads were awarded pay rises totalling £20m last year, with the salaries of some vice-chancellors almost doubling, research by The Times Higher Educational Supplement found.
In his final year as the Open University's vice-chancellor, Sir John Daniel's earnings more than doubled to £309,000.
The second-highest earner was John Quelch, of the London Business School, who was paid £308,000. He was followed by Sir John Kingman, the former vice-chancellor of Bristol University, whose pay rose by almost 100 per cent to £252,000 in his last year in the job.
Baroness Warwick, the chief executive of Universities UK (formerly the Committee of Vice-Chancellors and Principals), defended the pay rises.
She said: "Vice-chancellors' pay is a matter for individual universities. But, clearly, universities will wish the salaries of their vice-chancellors to reflect the fact that they are successfully running multi-million-pound businesses."
However, Sally Hunt, the assistant general secretary of the Association of University Teachers, said that the vice-chancellors' wealth contrasted with the poor pay of their staff.
The £20m awarded to vice-chancellors would have employed nearly 1,000 new university lecturers, the union said, with the average starting salary for a lecturer at little more than £20,000.
Ms Hunt said: "Yet again we have seen the fat-cat mentality of university vice-chancellors triumph over prudent and efficient management. It will be difficult for vice-chancellors to sustain the argument that lecturers and other university staff cannot have a decent pay increase this year when they have presided over such a large boost for themselves.
"The total pay increase for vice-chancellors is the equivalent of nearly 1,000 lecturers. During a period of underfunding and cutbacks, staff and students will be left bewildered by the insensitivity of vice-chancellors in this latest pay award."
Martin Ince, the deputy editor of The Times Higher Educational Supplement, said: "With resources across higher education under extreme pressure, it is difficult not to sympathise with poorly funded teaching staff and cash-strapped students, who will naturally be asking how these huge leaps in vice-chancellors' pay can be justified."