In this dissertation, I argue for the existence and critical relevance of a program of experimental literature in the long nineteenth century, developed in the aesthetics of German Romanticism and adapted in a set of texts by Thomas De Quincey, Charles Dickens and George Eliot. My introduction positions this argument in context of larger debates concerning form, theory and literary capacity, provides points of connection between these authors, and outlines the most prominent features of experimental literature. In the first chapter, I present an unorthodox reading of Kant’s Critique of Judgment, accompanied by a brief account of the literary-critical practice of the Athenaeum circle in Germany, as a means of establishing the philosophical values and theoretical underpinnings of the project of experimental literature. As Kant, Schlegel and cohort upheld ideals of beauty and literature grounded in unpredictable productivity and experimentation, De Quincey, Dickens and Eliot produced texts that seek to realize unanticipated connections in thought and sensation, following lines of association and speculation. Next, I argue that De Quincey’s depiction of Kant as producer of accumulative sentences and texts can provide a useful means of reading the literary experiments of Confessions of an English Opium-Eater and for complicating critical accounts of De Quincey’s hostility to Kant. In the third chapter, I read Dickens’s less-known Sketches by Boz and Mudfog Papers as instances of social, scientific and speculative experimentation that deserve to be read in their own light, rather than as anticipations of his novels. In the last chapter, I again offer experimental literature as a means of theorizing literary significance in the eccentric works of a novelist, with Eliot’s “The Legend of Jubal” and Impressions of Theophrastus Such. Far from reproducing an image of a natural and sympathetic realist, in these texts Eliot pursues vagrant lines of literary speculation and cultivates critical difficulty. Taken together, these literary and philosophical texts present an ideal and practice of experimental literature that prioritizes speculation over didacticism, the play of thought and language over their habitual use, and the exercise of criticism, analysis and humor over the veneration of the received and familiar