Smith was also one of the few Student Nonviolent Coordinating Committee workers employed in the original Head Start program.

Smith worked with native Mississippi sharecroppers who had been evicted from their homes when they requested a pay raise in the men's salaries from a flat rate of $6.00 per day to $1.25 per hour.

The sharecroppers, Frank and his first wife, Jean Smith, purchased land, lived in tents where they were regular and ongoing targets for the plantation owner and friends during the year when they built housing, and established one of the first (and only) black cooperative communities in Mississippi—Strike City.

As part of Freedom Summer, Smith and Frank Soracco, another Student Nonviolent Coordinating Committee worker, traveled the United States to raise funds for travel and expenses for the Mississippi Freedom Democratic Party and his friend and colleague, Fannie Lou Hamer to attend the 1964 Democratic National Convention.

While on the Council, he served as chair of the Housing and Economic Development Committee, the Washington Metropolitan Area Transit Authority, and the Baseball Commission.

Smith's office records from his time as a District council member are under the care of the Special Collections Research Center at the George Washington University.

Smith is the founding executive director and board member of the African American Civil War Memorial Freedom Foundation and Museum.