The jobless total, which includes people who are out of work and not eligible for benefits, increased by 7,000 over the quarter from June to August and is 10,000 more than it was at the same time last year.
That situation north of the border is in contrast with the UK as a whole, where unemployment fell by 50,000 over the same period to 2.53 million, the lowest since the spring.
The Scottish unemployment rate of 8.2% remains higher than the 7.9% rate for the UK as a whole.
It is the second month in a row unemployment in Scotland has increased, after a number of months when the jobless total had been falling.
The figures also showed that the number of Scots in work decreased slightly over the period from June to August.
The employment total dropped by 1,000 to 2,490,000 - although this is 16,000 higher than the same period last year.
Meanwhile the number of Scots who are out of work and claiming jobseeker's allowance fell by 1,300 from August, to stand at 139,900 in September.
Scottish Secretary Michael Moore said the rising unemployment level north of the border was "cause for concern".
But he said there were some "positive signs", highlighting the third consecutive fall in the numbers of people claiming jobseeker's allowance.
Mr Moore said: "Any increase in Scottish people losing their jobs is disappointing and a cause for concern across both Scotland's governments.
"Unemployment has a major impact on families and communities and our priority is to create opportunities to help people back into work. These are difficult economic times in the face of a world economy facing a number of challenges."
He said the UK Government's position was "consistent and clear that there can be no complacency in getting people back into jobs" as he stressed ministers were taking "decisive steps to deal with the UK's debt and deficit".
Mr Moore said: "The action we have taken so far has helped to make the whole of the UK, including Scotland, one of the most competitive economies."
He continued: ""There are some positive signs, such as the third consecutive monthly fall in the number of people claiming jobseeker's allowance.
"We will continue to do as much as we can to help people find work through targeted support available at Scotland's JobCentre Plus network."
The unemployment figures were released at the same time as the latest Gross Domestic Product (GDP) statistics showed Scotland had failed to emerge from recession.
And Deputy First Minister Nicola Sturgeon said: "We could not have a clearer example of why Scotland needs the full powers of independence."
Ms Sturgeon said the organisers of the London Olympics had estimated that more than 100,000 employment opportunities were created as part of the sporting event.
Ms Sturgeon said that for the UK figures "these jobs may have a masking effect on the reality of the economic situation".
She went on: "The UK Government must not be complacent - it is still clear that what is needed is a direct capital investment stimulus to boost the economy.
"Today's figures show once again that Scotland is suffering under the UK Government's do-nothing economic policy."
The Scottish Government has repeatedly urged the Tory-Lib Dem coalition at Westminster to provide funding for major capital investment projects to help boost the economy.
Grahame Smith, general secretary of the Scottish Trades Union Congress (STUC), hit out at the UK Government "damaging" austerity programme.
But he also called for the Scottish Government to "reappraise its policy agenda" to see how effective it was with unemployment rising.
Mr Smith said: "Once again, the statistics provide no cause for optimism that an end to this unprecedented and prolonged slump is in sight. Indeed, the coalition's damaging, unnecessary and ultimately self-defeating austerity project practically guarantees that the economic misery currently being visited on the Scottish people will persist for some considerable time.
"As the performance of the Scottish labour market deteriorates relative to the rest of the UK it will also be necessary for the Scottish Government to reappraise its policy agenda to determine its true effectiveness in defending jobs in the current climate."
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