He was a long-time member of North Street A.M.E. Church. Jaymes served on the first Board of Directors of the Center Street YMCA (a safe haven for young Black people), on the Board of Trustees at Wilberforce University, and as a Grand Chancellor of Ohio for the Grand Lodge, Knights of Pythias. During his distinguished legal career in Springfield, Jaymes held briefs in cases such as that of Richard Dixon, the lynching victim of Springfield’s 1904 race riot, and that of several African Americans indicted in the 1906 and 1921 race riots.

He played a prominent role during tense community discussions around school segregation at Fulton Elementary School. Jaymes helped lead the unsuccessful effort to stop the 1921 screening of Birth of a Nation at Springfield’s Memorial Hall. When Grace Bayless, a white woman accused of first-degree murder and facing the death penalty, requested Jaymes be appointed her defense attorney, the judge making the appointment in 1937 stated, “The Court considers this request as a tribute to your ability and influence before our courts and juries.” Sully Jaymes died on 20 January 1950.