The proportion of income that Premier League clubs spend on wages hit a record 68% in 2009-10, a report into football finances by Deloitte says.
While Manchester United spent 46% of its revenue on pay, rivals Manchester City splashed out a massive 107%.
Chelsea again topped the wages bill, as they have done every season since 2002-03, at £174m.
"This new high is worrying, something Uefa's financial fair play rules should address," said Deloitte's Dan Jones.
It comes as the Deloitte report shows Premier League revenues increased by 2% to exceed £2bn for the first time in the 2009-10 season.
Mr Jones said there were signs of wage discipline in clubs near the bottom of the Premier League, while those near the top earned such large revenues that it helped them keep the wage ratios down.
"The problem is with the middle tier of clubs, those who are neither chasing a Uefa place or facing relegation," said Mr Jones.
"And of course Manchester City and Chelsea are going to need to get wages under control for the financial fair play rules."
Those rules, which encourage football teams to balance revenues and costs, will start taking account of clubs' finances from next season.
To obtain a Uefa licence to play in the Champions League or Europa League, a club has to meet those break-even financial requirements.
"While football's revenue performance has been spectacular, sustainably managing its costs remains football's primary business challenge," Mr Jones said.
The "relentless growth in wages" has resulted in operating margins in the top division falling from 16% to 4% over the lifetime of the Premier League.
And other challenges remain - including debt, warnings from the government about football governance, and continued interest from tax and revenue authorities.
Meanwhile, the overall operating losses for the top four divisions in England now outstrip the Premier League's profits.
The 92 league clubs as a whole lose money on their day-to-day operations - and at the pre-tax level, losses have continued to grow, hitting £600m in 2009-10.
Collective club debts now stand at around £3.5bn.
On the wider European picture, each of the "big five" leagues - England, Germany, Italy, Spain and France - increased total revenues to record levels in 2009-19, reporting collective revenue of 8.4bn euros (£7.5bn).
TOP PREMIER LEAGUE WAGE BILLS 2009-10
- Chelsea - £174m (£167m)
- Man City - £133m (£83m)
- Man Utd - £132m (£123m)
- Liverpool - £121m (£107m)
- Arsenal - £111m (£104m)
Source: Deloitte, 2008-09 wage bills in brackets
It must be fantastic to earn that kind of money and love the job you do, although we think it has got ridiculous the amount players are paid. Says Greengates Builders Merchants Accrington, Lancashire.