Complications arise when the predictions of these "defect behavior" are extremely attuned to the atomic configuration of defects, and yet traditional modelling approach based on local optimization is subjected to false identification of the metastable vs. true ground-state atomic configuration. The big problem in surface catalysis modelling therefore, is the lack of sufficient quantum-chemical investigations with comprehensive, rigid, and accurate protocols based on wellgrounded theoretical framework for the proper identification of correct defect geometries. False identification of the true defect geometries will severely impact the theoretical predictions of materials' performance, including but not limited to catalytic activity, reaction selectivity, dopants concentration, and equilibrium concentrations. This Comment aims to highlight the false identification issue of defect geometries to the attention of catalytic community. We first introduce the common errors in surface defect modelling for contemporary a priori-driven catalysis research (i.e., first principles calculations), as even a minute change in the formation energy of a point defect may result in the predicted activation energy and reaction pathway to deviate greatly due to the several orders of magnitude fluctuations in the calculated defect concentration owing to the butterfly effect. We then provide a consolidated outline of the causes and potential impacts of the false identification and discuss frontiers computational approaches to address the big problem.