Soon after, however, when he was placed on half-pay, Moore decided to accompany his brother in law, John Wylde, who had recently been appointed Judge advocate of New South Wales, to Sydney, They arrived on 5 October 1816, on a ship called the Elizabeth, with Wylde making his official landing in the Governor's barge under a salute of thirteen guns on October 12.

In 1824 the Supreme Court of New South Wales was formally established, and Moore spent some time acting as a prothonotary, until the following year, when his post was abolished.

Two years later, Moore married Ann Augusta, daughter of Lieutenant John James Peters, with whom he had four children: two girls and two boys.

Among other things, Moore also took out, in October 1824, a ticket-of-occupation for over 2000 acres (8 km2) of land in an area where Canberra now exists, and in December 1826, he applied to buy some 1000 acres (4 km2) of land that he already occupied for over 3 years, 'situate at Canberry, on the E. bank of the river which waters Limestone Plains, above its junction with the Murrumbeeja, adjoining the grant of Mr Robert Campbell snr'.

"[1] Moore is known to have been the first pastoralist to ever occupy the land where Canberra, the capital of Australia, is situated presently, preceding Robert Campbell by approximately one year.