Baird was ordained minister of Dunkeld in 1787, and was appointed minister of Greyfriars Kirk, Edinburgh in 1792. In the same year he became Joint Professor of Oriental Languages in University of Edinburgh. In 1793, aged 33, he was appointed Principal of the University, and served in this role until 1840. In 1800 he was living at Ramsay Gardens at the top of the Royal Mile in Edinburgh. His election to a prominent position was said to be a result of the influence of his father-in-law, Thomas Elder of Forneth, the Lord Provost of Edinburgh, whose eldest daughter had married Baird some years previously. It is reputed to have been jocularly said that Baird's chief claim to the Principalship was as "Husband" of the Lord Provost's daughter. Nevertheless, Baird held the Principalship for the long period of 47 years. The number of students at the University increased from 1,000 to 2,000 while he held this position and the Old College buildings were completed. In 1810, before these new buildings were built, it was reported that 24 professors shared 11 rooms and two professors had to teach by candlelight even in the middle of the day. In 1800, Baird was chosen as Moderator of the General Assembly of the Church of Scotland. Baird was the founder and first convenor of the Highlands and Islands committee of the General Assembly. While on this committee he got the General assembly to agree to his project to educate the poor people in the highlands and islands of Scotland - in particular the Celts.
Later years
Towards the close of his life, Baird put much effort into a scheme for the education of the poor in the Highlands and Islands of Scotland. He submitted his proposals to the General Assembly of the Church of Scotland in May 1824. Next year the Assembly gave its sanction to the scheme, and it was launched most auspiciously. So intense was his interest in this work that in his 67th year, although in enfeebled health, he made frequent trips to many Highland destinations. Through his influence Dr Andrew Bell, of Madras, bequeathed £5000 for education in the Highlands of Scotland. Baird was also known as a correspondent of the Scottish poet Robert Burns. After his wife Isabella's death, Baird lived with his daughter Marion and son-in-law Isaac Bayley at 13 Regent Terrace, Edinburgh from 1827. He died here in 1840, and is buried a short distance from the house, at New Calton Cemetery. A memorial also exists near his family property at Manuel, in Muiravonside Churchyard.