This study introduces a new perspective on the design pedagogy in learning symbol design. A new experimental discipline implemented by the design methods demonstrates positive learning outcomes for students on the development of symbol study. Understanding denotative and connotative interpretation in visual literacy is essential in order to convey not only a clear message but also distinctive recognition as the nature of symbol quality. Students executed design experiments with design theories and methods for understanding design fundamentals of the denotative symbol and explored a matrix table for cultivating connotative symbols. This pedagogical strategy applied to the expansion of visual concepts with progressive experiments on each stage; 1) analyzing perceptive characteristics, 2) simplifying visual construction, 3) developing a visual concept with connotative meaning, and 4) configuring visual balance and enhanced quality based on design principles. With examples of student outcomes, this paper explains an analysis of functional expression and interpretation applied by design methods. This study discovered that earlier teaching of design fundamental disciplines with theories and methods in the graphic design major gave students better opportunities to pursue their further study more effectively and productively.