Elizabeth Schuyler Hamilton developed a sustained public role in charitable work and in preserving the record of Alexander Hamilton's life. During their marriage she managed a large household whose circumstances were closely connected to his military, legal, and political career. After his death in 1804 she faced debts supporting their children. She sought assistance and pursued claims arising from his public service while working to preserve his papers and defend his reputation.

In 1806 she joined other women in founding the Orphan Asylum Society of the City of New York. The organization provided a home, education, and practical support for children without parental care. Hamilton's contribution involved continuing administration and fundraising, not simply lending her name at its establishment. She served as second directress and later as first directress, remaining involved for decades. The institution evolved into the organization now known as Graham, whose history identifies her among several founders rather than as its sole creator.

Her charitable interests also included education for children whose families could not afford schooling. She supported a school in the Washington Heights neighborhood near the Hamilton family home. She joined networks of women providing assistance where public aid was limited, finding donors and sustaining institutions.

Hamilton also devoted substantial effort to gathering and safeguarding her husband's correspondence and other documents. She encouraged former associates to supply recollections and supported her son John Church Hamilton's work on his father's biography and writings. These efforts helped establish the documentary foundation through which later readers encountered Alexander Hamilton's public career. In old age she lived in Washington and supported commemoration of the Revolutionary generation. She died in 1854, having outlived her husband by fifty years and maintained an independent record of institutional service.