Ian Craig, boss of Lothian Buses, has been paid more than £1 million in the past five years.
Figures revealed that his pay package totalled £269,000 last year, including a bonus of £73,400 - more than either First Minister Alex Salmond or Prime Minister David Cameron. In the previous year, Mr Craig made £264,000 - an increase of £5100.
Kezia Dugdale, Labour MSP for Lothian, said: "Cleaners and care workers and others will look at these figures and think, there's one rule for them and another for the rest of us.
"People will find it hard to stomach that the man in charge of the trams and buses earns more than the Prime Minister and the First Minister."
Lothian Buses said Mr Craig's pay boost was justified because 2013 had been the company's most successful year in recent history.
Mr Craig is the chief executive of Transport for Edinburgh, which takes in Lothian Buses, Edinburgh Bus Tours and Edinburgh Trams.
Details of his salary and bonuses have only been published since 2011. His generous pay package increased from just over £209,000 in 2011 to £264,000 in 2012 and £269,000 last year, adding up to more than £743,000.
Figures for the previous two years, understood to have been around £200,000, put him over the £1 million mark.
Mr Craig came under fire last year over a 26% pay rise at a time when bus drivers had to settle for an increase of around 2%.
Lothian Buses' other three most senior staff were awarded rises of more than £3000 each, taking their packages to just below £200,000.
The company insist the pay hike was justified because it reflected increased responsibilities and positive performance.
In a statement, Mr Craig said: "We can demonstrate first-rate financial performance, engineering and operational quality, as well as a new tram operation which has been developed and delivered in time for service."
Lothian Buses had revenues of more than £132m last year, up £10m on the previous year, and net profit was £8.5m, an increase of 7.8% over 2012.
The company recorded 115m journeys last year - four million more than in 2012, and the highest recorded for over 25 years.
Ann Faulds, chair of Lothian Buses board, said: "I'd like to congratulate our CEO, Ian Craig, and his team for what they have achieved."