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Although the Next Generation Science Standards (NGSS) present a detailed set of Science and Engineering Practices, a finer grained representation of the underlying skills is lacking in the standards document. Therefore, it has been reported that teachers are facing challenges deciphering and effectively implementing the standards, especially with regards to the Practices. This analytical study assessed the development of high school chemistry students’ (N = 41) inquiry, multivariable causal reasoning skills, and metacognition as a mediator for their development. Inquiry tasks based on concepts of element properties of the periodic table as well as reaction kinetics required students to conduct controlled thought experiments, make inferences, and declare predictions of the level of the outcome variable by coordinating the effects of multiple variables. An embedded mixed methods design was utilized for depth and breadth of understanding. Various sources of data were collected including students’ written artifacts, audio recordings of in-depth observational groups and interviews. Data analysis was informed by a conceptual framework formulated around the concepts of coordinating theory and evidence, metacognition, and mental models of multivariable causal reasoning. Results of the study indicated positive change towards conducting controlled experimentation, making valid inferences and justifications. Additionally, significant positive correlation between metastrategic and metacognitive competencies, and sophistication of experimental strategies, signified the central role metacognition played. Finally, lack of consistency in indicating effective variables during the multivariable prediction task pointed towards the fragile mental models of multivariable causal reasoning the students had. Implications for teacher education, science education policy as well as classroom research methods are discussed. Finally, recommendations for developing reform-based chemistry curricula based on the Practices are presented.