The latest figures, covering the period May to July, showed an increase of 19,000 in the jobless total - up by 20.6 per cent on the previous three months.
Meanwhile, the number of Scots in work fell by 33,000 over the quarter to 2,669,000.
The employment rate among the working age population - those aged between 16 and 64 - fell by one percentage point from the previous quarter to 74.9%
In contrast across the UK employment rate was measured at 76.1% - the joint-highest total since comparable records began in 1971.
As well as having a lower employment rate than the UK, the figures, published by the UK Office for National Statistics, showed Scotland now has a higher unemployment rate.
In Scotland, the unemployment rate was 4%, compared to 3.8% in the UK as a whole.
The number of men out of work rose from 51,000 in the February to April to 62,000 in May to July.
There was also a rise in female unemployment over the period, from 40,000 to 48,000.
Scottish Secretary Alister Jack said: “It is disappointing to see a sharp increase in unemployment after a period of encouraging figures.
“It shows we cannot be complacent. One of our key priorities is to work with the Scottish Government to boost the Scottish economy and create jobs.
“The UK Government is investing £1.4 billion in city and growth deals and we are preparing to take advantage of the opportunities that will arise when we leave the EU on October 31.
“But I would urge the Scottish Government to use their powers to best effect.
“Making Scotland the highest taxed part of the UK and creating uncertainty by threatening a second independence referendum are holding Scotland back.”