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Mitchell became of the first importance. After ascending the Murray to near its junction with the Goulburn, he turned off to the south-west, drawn in that direction by the fine quality of the country. The region he thus opened up was called by him Australia Felix, and it no doubt forms one of the richest tracts in Australia. Continuing his journey in this direction, he struck the Glenelg, as he named it, after the colonial secretary, Charles Grant, lord Glenelg [q. v.], and followed it to the sea. At Portland Bay he found one solitary settler, Edward Henty [q. v.] He returned to Sydney by a route parallel to that of his advance from the Murray, but nearer to the sea. Here he soon came into country more or less known through the travels of Hovell and Hume, and near where Albury now stands. He found the country on the eve of being taken up by colonists. This journey, which lasted over seven months, thus added greatly to the knowledge of a very fertile region of Australia.

Mitchell went on leave to England in 1839, and the value of his services was recognised by his being knighted, and he received the honorary degree of D.C.L. at Oxford. He returned to Australia in 1840, and was promoted to the rank of lieutenant-colonel on 23 Nov. 1841. In 1844 he was elected as a member of council to represent Melbourne, but on its being indicated to him that his vote as government officer was required by the government, he resigned his seat.

The dangers attendant on the navigation of the Torres Straits made it appear very desirable to open an overland route to the gulf of Carpentaria, especially with the view of facilitating the trade in horses with India. Mitchell's fourth expedition was undertaken with the object of ascertaining if a practical road could be found. He left Sydney in November 1845, accompanied by E. B. Kennedy as second in command, and by W. Stephenson as naturalist. He first ascended the valley of the Narran, a river which had quite recently been discovered by his own son; then, entering quite unknown land, he traced the Maranoa up to close to its source, and thence struck across more difficult country to the head waters of the Belyando. After tracing this river for some two hundred miles towards the sea, and after coming to the conclusion that it must join the Siittor river of Leichhardt [q. v.], he retraced his steps to the Belyando. Hence he struck out again in a north-westerly direction, and discovered the sources of the Barcoo. He felt certain—but in this he was in error—that this must be the great river flowing into the gulf of Carpentaria, along the banks of which the great road to the north would be found. He traced the Barcoo to within a few miles of the point where it turns in a south-westerly direction, and he thus found nothing to shake the confidence of his belief. This was his furthest point, and he returned to civilisation in January 1847, after an absence of over a year.

Despite Mitchell's mistaken supposition, this last journey only served to confirm his high reputation as an explorer. On all his expeditions, which made great additions to Australian botany, he was accompanied by a comparatively large number of followers, (twenty-nine men on the last occasion), and all the details were carefully thought out beforehand. The rank and file of his expeditions always consisted of convicts, who almost invariably did good service in the hope of a free pardon as a reward; but that such men should have been led for so many months without any serious disturbance must be attributed to the personal qualities of their chief. A man of great personal courage, he had a somewhat imperious manner and temper, and spoke out so fearlessly that he made many enemies. He was evidently impressed with a strong sense of justice towards the natives and hated cruelty to animals. In 1851 he was sent to report on the Bathurst goldfields. He again visited England in 1853, and patented a new screw-propeller for steam-vessels called the 'Boomerang,' respecting which he published a lecture delivered at the United Institution. He died at his house, Carthona, Darling Point, 5 Oct. 1855. The cause of his death was variously attributed to worry concerning an inquiry that was being held on the department under his charge, or to exposure while on his last expedition. He married in 1818 a daughter of Lieutenant-colonel Blunt. His son Roderick (1824-1852) was engaged in surveying to the north of New England (New South Wales), and was appointed to the command of the expedition in search of Leichhardt, but was drowned on the passage from Newcastle.

Mitchell, a fellow of the Royal and Geographical Societies, was a man of much literary culture. He published a technical work, 'Outlines of a System for Geographical and Military Purposes,' 1827, besides two volumes recounting his explorations, which, though accurate and painstaking, somewhat reflect the monotonous character of the country and of the methods of travel described. Their titles ran: 'Three Expeditions into the Interior of Eastern Australia, with Description of the recently explored Region of Australia Felix, and of the present Colony of New South Wales,' London, 1839; '