This thesis identifies and explains the gaps in prior and current applications of representational competence construct in chemistry. Representational competence (RC) describes a set of skills that chemistry researchers Kozma and Russell observed experts demonstrate when engaging with disciplinary representations (Kozma & Russell, 1997; Kozma & Russell, 2005). These skills have commonly been used as a frame for other researchers to study student engagement with disciplinary representations and to design instructional practices to improve novice skill development. A comprehensive review of the literature that invokes representational competence, both within and without the domain of chemistry, has led to the characterization of several concerns regarding how the RC construct has been applied theoretically and empirically. These concerns include inconsistencies between RC skill definitions, the appropriateness of using RC to evaluate novices, the varied instruments used to measure RC, lack of alignment between targeted RC skills and measurement tools, and the minimal or non-existent correlation between RC and content knowledge. I conducted two separate studies that utilize a more comprehensive and cognitive-focused approach to analyzing student engagement with chemistry representations to address the concerns apparent in current RC research. I also suggest multiple alternative theoretical frameworks that can be applied to RC studies in order to create a more robust and detailed characterization of how students understand and learn with different chemistry representations. [The dissertation citations contained here are published with the permission of ProQuest LLC. Further reproduction is prohibited without permission. Copies of dissertations may be obtained by Telephone (800) 1-800-521-0600. Web page: http://www.proquest.com/en-US/products/dissertations/individuals.shtml.]