Strategies for teaching NMR spectral interpretation in the undergraduate organic chemistry curriculum are often faculty-centered and can lead to student reliance on rote memorization and "guess and check" methods rather than critical-thinking skills for structure determination. This article describes a student-focused methodology for the introduction of NMR spectral interpretation. Guided-inquiry tutorials using NMR prediction tools were developed to enable students to investigate the trends and concepts in [superscript 13]C and [superscript 1]H NMR spectral interpretation, with an emphasis on making connections between data and foundational chemical knowledge. A systematic approach to solving unknown structure problems is presented, providing a framework for students to organize spectral data and to build molecules from partial structures. The success of this NMR spectroscopy teaching strategy, which can be adapted for either laboratory or lecture environments, was demonstrated both in positive student survey responses as well as in quantitative data showing a significant improvement in exam question scores.