In the silicone material extrusion (MEX) process, product profile error and performance defects are common problems due to changes in strand shape. A process optimization method considering strand morphology, denoted as SMO, which allows adjustment of the strand shape by adjusting process parameters during the printing process is presented. The relation between process parameters (extrusion speed, moving speed, nozzle height, and nozzle radius) and the geometric parameters (strand width and strand height) of the cross-section, as well as the relationship between strand spacing, layer height, and process parameters in no void constraint is discussed and verified. SMO was utilized to produce specimens with tunable strand width and strand height. Tensile tests and profile scans were performed to compare SMO with other methods to verify its feasibility. Specimens fabricated using the SMO method have up to a 7% increase in tensile strength, up to a 10% reduction in processing time, and about a 60% reduction in strand height error over unused ones. The results show that the SMO method with adjustable strand width can effectively balance efficiency and mechanical properties compared to uniform infill, and the SMO method with adjustable strand height can provide higher accuracy compared to uniform strand height. The proposed method is validated and improves the efficiency and accuracy of silicone MEX.