A fishing community was established on the island in the 1800s, and at one time there were about 300 residents living primarily at two locations: Mercer's Cove and Forward's Cove.

[3][4] In 1964, an experimental attempt to introduce bison to Newfoundland was made, using Brunette Island as a test site; the attempt did not prove successful;[5][6][7] the rocky landscape and sheer cliffs on the island were significantly different from the wide plains to which the bison were adapted.

[8] With more success, wildlife biologists continued to use Brunette as a site for wildlife observation and a breeding ground for Arctic hare, caribou, ptarmigan, and moose.

[10][11] From October 12–23, 2016, Mack McGowen, a native of Tyler, Texas, lived alone on Brunette Island and streamed the experience live on Facebook in a documentary titled "Castaway Live.

"[12] Mercer Head on Brunette Island continues to be the site of a navigational light.