The structure elucidation of organic molecules through 1D and 2D nuclear magnetic resonance (NMR) data analysis is a potentially challenging, combinatorial problem. Our new publication presents Sherlock, a free and open-source Computer-Assisted Structure Elucidation (CASE) software where the user controls the chain of elementary operations through a versatile graphical user interface, including spectral peak picking, the addition of automatic or user-defined structure constraints, structure generation, ranking and display of the solutions.