Some 794 new complaints about the £2.8 billion industry were received in the financial year 2013/14 compared with 296 in 2011/12, and the service warned these cries for help are likely just the "tip of the iceberg".
The ombudsman fears the stigma associated with payday loans is preventing many more people who use them from seeking its help.
The most common reason for someone making a complaint about a payday loan is that they are being chased for a debt they never took on in the first place, the ombudsman said.
Often this is due to fraudsters successfully applying for a payday loan by using another person's identity.
The volume of payday loan borrowers bringing a complaint to the Financial Ombudsman Service is still tiny compared with more than 66,500 people who sought help with payday loan debt from the charity StepChange last year.
Nearly two out of every three (63%) complaints about payday lenders are resolved by the ombudsman in the consumer's favour.
The payday lending industry is currently undergoing a competition investigation. The Financial Conduct Authority, which took over supervision of the sector in April, has been phasing in a clampdown on the lenders amid widespread concerns that some borrowers have found themselves caught in a debt spiral.