Charles Peirce (1839-1914) was one of the most important logicians of the nineteenth century. This thesis traces the development of his algebraic logic from his early papers, with especial attention paid to the mathematical aspects. There are three main sources to consider. 1) Benjamin Peirce (1809-1880), Charles's father and also a leading American mathematician of his day, was an inspiration. His memoir Linear Associative Algebra (1870) is summarised and for the first time the algebraic structures behind its 169 algebras are analysed in depth. 2) Peirce's early papers on algebraic logic from the late 1860s were largely an attempt to expand and adapt George Boole's calculus, using a part/whole theory of classes and algebraic analogies concerning symbols, operations and equations to produce a method of deducing consequences from premises. 3) One of Peirce's main achievements was his work on the theory of relations, following in the pioneering footsteps of Augustus De Morgan. By linking the theory of relations to his post-Boolean algebraic logic, he solved many of the limitations that beset Boole's calculus. Peirce's seminal paper 'Description of a Notation for the Logic of Relatives' (1870) is analysed in detail, with a new interpretation suggested for his mysterious process of logical differentiation. Charles Peirce's later work up to the mid 1880s is then surveyed, both for its extended algebraic character and for its novel theory of quantification. The contributions of two of his students at the Johns Hopkins University, Oscar Mitchell and Christine Ladd-Franklin are traced, specifically with an analysis of their problem solving methods. The work of Peirce's successor Ernst Schröder is also reviewed, contrasting the differences and similarities between their logics. During the 1890s and later, Charles Peirce turned to a diagrammatic representation and extension of his algebraic logic. The basic concepts of this topological twist are introduced. Although Peirce's work in logic has been studied by previous scholars, this thesis stresses to a new extent the mathematical aspects of his logic - in particular the algebraic background and methods, not only of Peirce but also of several of his contemporaries.