In this study we propose a four-stage approach, which includes data envelopment analysis, Malmquist productivity index (MPI), entropy method and grey relation analysis (GRA), to investigate the operational performance of six thin film transistor liquid crystal display (TFT-LCD) companies in Taiwan during 2009–2012. The input variables are fixed assets, operating expenses, R&D expenses and number of employees, while the output variables are cash flow and net sales. The empirical results showed that companies AUO and HannStar could increase their operation efficiency by improving their VRS efficiency and scale efficiency. When using the MPI model to measure the productivity changes for these TFT-LCD companies, we found that the technology changes in most of the companies are downward tendencies during 2009–2012 except for Ampire. Thus, not only could the proposed GRA with entropy weights evaluate the current performances of each firm effectively, it can also predict their future performances.