Although raised in Charleston, South Carolina, Angelina and Sarah spent their entire adult lives in the North. Angelina's greatest fame was between 1835, when William Lloyd Garrison published a letter of hers in his anti-slavery newspaper ''The Liberator'', and May 1838, when she gave a speech to abolitionists with a hostile, noisy, stone-throwing crowd outside Pennsylvania Hall. The essays and speeches she produced in that period were incisive arguments to end slavery and to advance women's rights.
Drawing her views from natural rights theory (as set forth in the Declaration of Independence), the United States Constitution, Christian beliefs in the Bible, and her own childhood memories of the cruel slavery and racism in the South, Grimké proclaimed the injustice of denying freedom to any man or woman. She was particularly eloquent on the problem of racial prejudice. When challenged for speaking in public to mixed audiences of men and women in 1837, she and her sister Sarah fiercely defended women's right to make speeches and participate in political discourse.