[5] Sherrod first took part in the civil rights movement after the Supreme Court of the United States desegregated public schools in the Brown v. Board of Education case.

[5] He was a key member and organizer of the Student Nonviolent Coordinating Committee (SNCC) during the civil rights movement.

[5] In 1961 he was among four students, along with Diane Nash, J. Charles Jones, and Ruby Doris Smith, to drop out of college to become full-time civil rights activists and members of SNCC.

Sherrod's strategy was to focus on the small town of Albany, Georgia as the hub for voter registration activity for the surrounding farm country.

[9] Rather than returning to school in the fall, Sherrod moved to become a full-time organizer to stimulate new black initiatives in the strongly segregated and Ku Klux Klan–dominated community of Albany, Georgia.

While Sherrod and Reagon emphasized direct action, including sit-ins and jail-ins, and held learning sessions on how to engage in nonviolent strategies for Albany students in anticipation of a major conflict with the police,[11] local leaders preferred negotiation with authorities for reforms.

While some local leaders, such as C. W. King, an African-American real estate agent, and H. C. Boyd, the minister at Shiloh Baptist Church, supported the campaign, others considered forcing Sherrod and Reagon to leave town.

[12] Sherrod, Reagon and SNCC were also at odds with the tactics employed by Dr. Martin Luther King Jr. and the Southern Christian Leadership Conference.

While the movement was based on the nonviolent methods Sherrod learned from King, Sherrod advocated a more democratic approach based on grassroots organizing and aimed at long-term solutions, rather than King's style of short-term campaigns, dependent on his personal charisma and featuring more top-down direction.

[9] Sherrod's direct action tactics met with determined opposition from the authorities, particularly the Albany police chief, Laurie Pritchett, who ordered mass arrests of demonstrators, but avoided the sort of overt violence that would draw national attention and support for the movement.

Sherrod participated in the Selma Voting Rights Movement, along with other activists such as Dr. King and John Lewis.

When Sheriff Jim Clark barred Blacks' efforts to register to vote the movement decided on a march from Selma to Montgomery, Alabama, the state capital, to publicize their cause.

A supporter of racial integration, Sherrod recruited white as well as Black members to assist with voter registration efforts.

He then started recruiting students from the Union Theological Seminary, where he had received his master's degree, to assist in the project.

[17] This project has three main focuses: food, farms, and human rights, working in conjunction with New Communities and land trusts.