The main purpose of this study is to compare Saussure's (Ferdinand de Saussure 1857-1913) Semiology with Peirce's (Charles S. Peirce, 1839-1914) Semiotics and discuss how to choose a theory appropriate for Visual Communication Design from Saussure's Semiology and Peirce's Semiotics. In order to achieve the purpose, in this study, first, documentary research was applied to obtain the major point of Saussure's Semiology and Peirce's Semiotics. Besides, comparative analysis was applied to compare and analyze the concepts between Saussure's Semiology and Peirce's Semiotics. Further, documentary research and comparative analysis were also applied to obtain the major points appropriate for the applications to Visual Communication Design from Saussure's Semiology and Peirce's Semiotics. The following are the findings of this study. First, there are many differences between Saussure's Semiology and Peirce's Semiotics. For example, Saussure's Semiology is based on the concepts of Associationistic Psychology and Sociology; but Peirce is an antipsychologism and his Semiotics is based on the Behaviorism developed from Pragmatism. Next, Peirce's Semiotics is more suitable for being an applied theory to Visual Communication Design, because Peirce's types of sign provide many models and methods to the designers in analysis for the works of Visual Communication Design. Last, there is no doubt that Saussure's Semiology is very important in some way. The theories of two called Semiotics. That means they have many similar views. Therefore, it might be hard to choose between Saussure and Peirce.