In 1889 Metcalf received a large bequest from his father's business partner, Henry J. Steere. Metcalf served as a member of the Rhode Island House of Representatives from 1889 to 1891 and in 1907, and was a member of the Providence Common Council from 1888 to 1892. He was chairman of the Metropolitan Park Commission of Rhode Island from 1909 to 1924, and a member of the penal and charitable board from 1917 to 1923.
Metcalf was elected as a Republican to the United States Senate on November 4, 1924, to fill the vacancy caused by the death of LeBaron B. Colt; on the same day he was also elected for the term commencing March 4, 1925. He was reelected in 1930 and served from November 5, 1924, to January 3, 1937; he was an unsuccessful candidate for reelection in 1936. He is the last Republican to date to hold Rhode Island's Class 2 Senate seat.
While in the Senate he was chairman of the Committee on Patents (Sixty-ninth and Seventieth Congresses) and a member of the Committee on Education and Labor (Seventy-first and Seventy-second Congresses).
He died in Providence in 1942; interment was in Swan Point Cemetery. The Jesse H. Metcalf Lodge at Camp Yawgoog, the funds for which were donated by his wife, houses the Camp Sandy Beach dining hall and was named in his honor. Metcalf's sister, Eliza G. Radeke, served as president of the Rhode Island School of Design from 1913 to 1931.
In the early 1920s, the logging of ancient Redwood Forests in Northern California nearly extinguished a primordial coastal redwoods (Sequoia sempervirens). A last ditch conservation effort to preserve a grove of these trees was undertaken following publication of a series of photographs showing the size of these ancient trees.
Within Jedediah Smith Redwoods State Park, within the Redwoods National Park, there is a plaque that reads the following:
"The Metcalf Grove
This Grove is Given to the State of California
for the
Preservation of these Ancient Trees
by
Mr. And Mrs. Jesse M. Metcalf
of Rhode Island"
Location: 41.765485, -124.129551