The statistics prompted an attack by First Minister Alex Salmond on Chancellor George Osborne for "complacency".
The UK's jobless total fell by 49,000 between July and September to 2.51 million, official figures showed.
But in Scotland the number of people who are unemployed - which includes those out of work and not eligible for benefits - increased by 4,000 to 218,000 over the same period.
The unemployment rate north of the border remains above that for the UK as a whole, standing at 8.1% compared to 7.8%.
As well as the rise in the jobless total, the number of Scots in employment fell by 27,000 between to July and September, to 2,472,000.
The Scottish employment rate is now now 70.6% - lower than the UK average of 71.2%
The number of people who are out of work and claiming jobseeker's allowance has also risen slightly north of the border. This increased by 100 from September to 140,700 in October.
Across the UK, unemployment has fallen to its lowest total for over a year, although there has been an increase in the number of people claiming jobseeker's allowance.
The jobless total dropped by 49,000 in the quarter to September to 2.51 million, the lowest figure since last summer.
But the so-called claimant count jumped by 10,100 last month to 1.58 million, the highest since July, and the biggest monthly rise since last September.
The number of people in work increased by 100,000 in the latest quarter to just under 30 million, a rise of over half a million over the past year.
Other figures from the Office for National Statistics showed that long-term unemployment - those out of work for over a year - increased by 12,000 in the quarter to September to 894,000, while 443,000 people have been jobless for over two years, up by 21,000.
Part-time employment increased by 49,000 to 8.1 million, close to a record high, while there were 51,000 more people in full-time jobs, at 21.4 million.
Unemployment among women fell by 10,000 to 1.09 million, and by 39,000 among men to 1.43 million.
Unemployment among 16 to 24-year-olds fell by 49,000, which accounts for the total fall in today's jobless figures.
More young people are classed as economically inactive, most of whom were in full-time education.
Average earnings increased by 1.8% in the year to August, up by 0.1% on the previous month, giving average weekly pay of £471, including bonuses.
First Minister Alex Salmond hit out at the UK Government, claiming the "complacency" of Chancellor George Osborne was the "biggest danger to the economy".
He accused the Westminster Government of "basking in the Olympics afterglow" while it was "still clear that what is needed is a direct capital investment stimulus to boost the economy".
Mr Osborne will deliver his autumn statement next month and Mr Salmond said the rising jobless figures meant it was "ever more critical" for him to "take meaningful action to bring jobs and growth to the UK economy".
Mr Salmond said: "The biggest danger to the economy is the complacency of George Osborne. He should remember that the positive effect of the Olympics on employment will only last a few months whilst the impact of the decisions he makes in this forthcoming autumn statement will last for years."
Mr Salmond said the number of people out of work and claiming benefits was "unchanged" across the UK over the last year.
He added: "It is time the Chancellor faced the reality that as a result of his decisions the UK's economy is flat-lining. It would be a tragedy for Scotland, and for the UK as a whole, if the positive impact of the Olympics is used to justify continued inaction by the UK Government.
"An extra £5 billion in capital investment across the UK would allow us to provide an additional stimulus of more than £400 million to support employment in Scotland now."
Scotland Office Minister David Mundell said it was a "cause for obvious concern that the latest Scottish figures show another increase in unemployment while it is falling in the rest of the UK".
He added: "The fact the Scottish unemployment rate is also higher than the rest of the country shows why Scotland's two governments need to work together for the benefit of Scotland."
The UK Government said that from next year Scottish Secretary Michael Moore would jointly chair a Scottish Employability Forum with Finance Secretary John Swinney and councillor Harry McGuigan, the health and wellbeing spokesman for local government organisation Cosla. This forum will bring together the government, employers and others to try to tackle the problem.
Mr Mundell said: "Today's figures are a reminder we must redouble our efforts to rebalance the economy and get people back into sustainable jobs. Each one of these statistics represents a person or a family affected by serious economic conditions across the globe and we must do all we can to help them."
Unemployment between July and September was:
Region Total unemployment Change on quarter % rate
Scotland 218,000 +4000 8.1%
Northern Ireland 67,000 +1000 7.6%
Wales 121,000 -5000 8.2%
North East 127,000 -7000 9.8%
North West 293,000 -26,000 8.4%
Yorkshire/Humber 247,000 -20,000 9.1%
East Midlands 178,000 -15,000 7.7%
West Midlands 235,000 no change 8.6%
East of England 212,000 +8000 6.8%
London 372,000 +6000 8.7%
South East 289,000 +6000 6.5%
South West 155,000 -2000 5.8%