Statistics show an 8% rise in the number of deaths between 2011 and 2012, increasing from 525 to 567.
Among this number, deaths from intentional self-harm in those aged 60 and over rose from 58 in 2011 to 90 in 2012.
Figures for 2013 were not included as they have not been finalised by the National Records of Scotland.
Liberal Democrat MSP Jim Hume said: "These sobering figures show just how important it is that people suffering with self-harm are receiving the support they need.
"Self-harm is clearly a complex issue and there are no quick fixes here. But what we must do is work to ensure that health services - particularly mental health services - are available to those who need them at the right time."
He added: "All too often mental health services are the poor relation of our NHS and currently a postcode lottery in access to crucial psychological therapies means that waiting times often have more to do with geography than clinical need.
"This needs to end, which is why Liberal Democrats have called for equality between mental and physical health care to be enshrined in law."