About one in ten looked for help from the NHS smoking cessation services, the Scottish Government said.
Women, including those who were pregnant, and older people were more likely to try to stop, with the largest number of people coming from “deprived” areas.
The number of quit attempts increased by 29% from 83,952 in 2010 to 108,268.
Public health minister Michael Matheson said: “2011 saw the largest-ever increase in Scots trying to stop smoking, which is the biggest single step anyone can take to improve their health.
“I welcome the fact one in 10 smokers - over 100,000 Scots - took advantage of NHS Scotland stop smoking services last year, with the largest number from our most-deprived areas.
“It is also encouraging to see the number of pregnant women trying to quit increasing by nearly 50%.”
Meanwhile, statistics also showed drug-related hospital discharges have risen to a five-year high.
The rate increased by 26% between 2006-7 and 2010-11, from 98 to 123 diagnoses per 100,000 of the population of Scotland.
Overall, there were 6,166 occasions when someone was admitted to hospital after taking drugs in 2011 - an increase of more than 400 on the previous year and much higher than the 4,834 who were admitted in 2007.
The increase contrasted with a 6% fall in the rate of alcohol-related discharges from a general acute hospital over the same five years.
The Scottish Government said some users had been taking substances for more than a decade, increasing the risk of ill-health and death.