Crisp and fuzzy optimization approaches were applied to design an optimal temperature and pH control policy for a batch process of simultaneous saccharification and co-fermentation (SSCF) for ethanol production from lignocellulose, using the enzyme and recombinant strain Zymomonas mobilis ZM (pZB5). To determine an optimal temperature and pH control policy, we applied the Arrhenius relationship to each rate constant to express the temperature and pH effects in the kinetic model for both saccharification and fermentation. The goal of the optimal design was to determine the optimal temperature, pH value, initial lignocellulosic concentration, and fermentation time for maximizing the ethanol productivity under the constraints of the follow-up separation specifications. The interactive crisp and fuzzy optimization methods were applied to solve the trade-off optimization problems for obtaining a compromised design. The fuzzy goal attainment approach obtained a compromised design more flexibly than did the crisp optimization. We also compared the performances for batch and fed-batch SSCF, and used various composition proportions for the batch SSCF to determine a series of optimal designs for the fuzzy goal attainment problem. Batch SSCF was slightly more effective than fed-batch fermentation, and spruce exhibited the maximum productivity because of its higher cellulose and lower hemicellulose contents compared with those of other sources.