A method for searching, analyzing, and optimizing process parameters and a computer product thereof are provided. At first, sets of process data that are generated when a process tool processes workpieces are obtained respectively, each set of process data including process parameters. Then, sets of metrology data measured by a metrology tool are obtained, wherein the sets of metrology data are corresponding to the sets of the process data in a one-to-one manner, each workpiece having at least one measurement point, each set of metrology data including at least one actual measurement value of at least one measurement item at the at least one measurement point. Thereafter, critical parameters are selected from the process parameters. Then, values of the critical parameters are adjusted to enable predicted measurement values of the measurement points of one workpiece to meet a quality target value.