[3][5] As the varsity quarterback, he led the City Knights to two undefeated seasons and successive Maryland Scholastic Association A-conference championships in 1965 and 1966.

Schmoke was elected president of the school's student government in his senior year but also worked in the Baltimore community with disadvantaged youth.

Compulsory community service had not yet been mandated for Baltimore high school students, yet he tutored and mentored young men from the inner city as a member of the Lancers Boys Club.

While at Yale, Schmoke and his classmates started a day care center on campus for the children of the university's janitors and cafeteria workers who lived in New Haven.

[9] Schmoke has been acknowledged as the undergraduate student leader who helped quell the possibility of riot on the Yale campus in the wake of the New Haven Black Panther trials in the spring of 1970.

"[10] This moment is credited with helping to dispel the growing tensions: the university voted to bend its rules, making classes "voluntarily optional" to the end of the term, and despite small outbreaks of violence, no campus-wide unrest resulted.

[13] In 1977, he was selected to be part of the White House Domestic Policy Staff during the Carter Administration to work in the Department of Transportation.

[13][14] After one year working in President Carter's administration, Schmoke returned to Baltimore as the Assistant United States Attorney, a position he held from 1978 to 1981.

[22] In 1992, President George H. W. Bush awarded him the National Literacy Award for his efforts to promote adult literacy and, in 1994, President Bill Clinton cited Baltimore's programs to improve public housing and enhance community economic development and named Baltimore one of six cities to receive Empowerment Zone designation.

An edited version of a transcript of that speech entitled, "Why School Vouchers Can Help Inner-City Children", is available online and in that brief web page, Schmoke explains why he believes [that] school choice and vouchers will improve the quality of public education for America's youth, particularly inner-city minority children.

The Compelling Need to Reform National Drug Control Policy" for the Edward Bouchet Conference on Diversity in Graduate Education at Yale University.

The episodes, entitled "Middle Ground" and "Mission Accomplished", featured Schmoke in a bit part as a health commissioner.

[4][32] On September 8, 2017, President Schmoke made the decision to have Department of Education Secretary Betsy DeVos as the Fall 2017 commencement speaker.

In January 2024, John P. Angelos reached a $1.725 billion deal to sell the Baltimore Orioles to a group led by David Rubenstein.