It follows a trend across England – where a record number of firefighters also left the industry last year – as unions remain embroiled in a pay dispute during the cost-of-living crisis.
The Fire Brigades Union said low pay alongside tighter budgets is to blame for workers leaving the industry.
Home Office figures show 67 full-time and on-call firefighters left the Surrey Fire and Rescue Service in 2021-22 – up from 54 the year before and the highest number since records began in 2009-10.
Across the country, 3,359 firefighters left their jobs last year – a 28% increase on 2,628 in 2020-21 and also a record.
Meanwhile, the total number of employees leaving the fire industry, which includes support and fire control staff as well as firefighters themselves, also reached a record high last year (4,640).
In Surrey, 17 other staff left in 2021-22, meaning a total of 84 employees left the fire service – the most since records began.
The FBU said pay across the industry must be addressed to prevent further departures, with many "unable to pay for their families' cost of living".
Matt Wrack, general secretary of the union, said no firefighters and control staff should have to use foodbanks or struggle to pay the bills.
"It is a totally disgusting state of affairs for us as a society," added Mr Wrack.
"We need to think seriously about increasing pay, or the numbers of people leaving will increase – and the quality of life of tens of thousands of the most important people in society will continue to decrease."
Early or normal retirement was the most common reason for leaving nationally, accounting for 35 per cent of all departing staff last year.
Meanwhile, 69% more staff resigned to take up alternative employment in 2021-22 than the year before.
Figures on fire service leavers cover the headcount, rather than the number of equivalent full-time workers – but FTE firefighters have also continued to decline across England.
Numbers fell for the 15th successive year to 31,100 as of the end of March, meaning there are now 27% fewer FTE firefighters across the country than in 2007, when there were 42,400.
Surrey had 543 FTE firefighters last year – though this was up from 530 the year previous.
Mr Wrack said tightening budgets are to blame for the declining numbers on a national scale.
"We cannot continue to have a situation where threadbare fire services are meant to keep our communities safe," he added.
"Firefighters and control staff need to get the proper resources to do their jobs; anything else lets firefighters and control staff down and lets the public down."
The Home Office said it has " consistently given fire services the resources they need to keep people safe", including £2.5 billion in funding this year.
"We are committed to working in partnership with chief fire officers to ensure the fire service is fit to face the demands of the future," a spokesperson added.