The ranks of Spanish job seekers swelled by 1.7 percent over the month to stand at 4.7 million in September, the labour ministry said Tuesday.
The number of Spaniards registered as seeking work increased by 11.3 percent from September last year.
In September, the number of jobless people mostly rose in the service industry -- up 85,713, while dipping slightly in the agriculture (down 2,633), construction (down 9,687) and industry (down 966) sectors.
According to the National Statistics Institute, which uses a different calculation, the overall unemployment rate had reached 24.63 percent by the end of June, a record in the industrialised world.
The government sees the jobless rate at 24.6 percent at the end of 2012, before dipping slightly to 23.3 percent in 2013.
According to a study published Monday by the UGT union, close to a million people have been looking for work for more than two years, or some 20.8 percent more than a year ago.
Spain has been struggling since a property market crash in 2008.
The government expects the economy to contract by 1.5 percent in 2012 and 0.5 percent in 2013 before returning to growth in 2014 with an expansion of 1.2 percent, and in 2015 with 1.9 percent.
But these forecasts are viewed as optimistic by the market. The International Monetary Fund estimates a contraction of 1.2 percent in Spanish GDP for 2013, while Standard and Poor's expects the economy to shrink by 1.4 percent. Bank Natixis has issued the most pessimistic forecast of a 2.2 percent contraction for the year.