In the summer of 1926 Gould undertook his first trip to the Arctic, serving as assistant director and geologist with the University of Michigan Greenland Expedition.

The following summer he was geographer and topologist for George P. Putnam's expedition to survey the coast of Baffin Island in Arctic Canada.

In March 1929 Gould along with Harold June and Bernt Balchen flew in the expeditions Fokker Universal east to establish a geologic camp near the Rockefeller Mountains at the edge of what would soon be known as Marie Byrd Land.

[2] On November 4, 1929, Gould and five companions began a grueling 2½ month, 1500-mile dog-sledge journey into the Queen Maud Mountains, with the primary purpose of providing ground support and possible emergency assistance for Byrd's historic first airplane flight over the South Pole and a secondary purpose of conducting the first geological and glaciological survey of an area that Gould called "a veritable paradise for a geologist.

The layered sandstones that Gould found in outcrops at the mountain's peak helped confirm that Antarctica was linked geologically to the Earth's southern continents in Gondwana.

On August 2, 1930, two weeks after returning from Antarctica, Gould married Margaret ("Peg") Rice in Ann Arbor, Michigan.

In 1932 Gould and his family moved to Minnesota after he accepted a position as a full professor at Carleton College where he founded and served as chairman of the geology department.

The R/V Laurence M. Gould, a 76-m-long ice-strengthened research ship built in 1997 for the National Science Foundation and designed for year-round polar operations, is named in his honor.