AbstractAdditive manufacturing of thermoplastic elastomers is challenging using fused deposition modeling due to their high melt viscosity, low column strength, and poor fusion among layers. Solvent‐cast 3D printing (SC‐3DP) is an efficient alternative to successfully 3D print such materials. However, selection of suitable 3D printing parameters is crucial to realize parts with optimum physicomechanical properties. In this work, statistical modeling and SC‐3DP parameter optimization for styrene–ethylene–butylene–styrene (SEBS) block copolymer were performed. The effect of 3D printing process parameters on shrinkage, relative density, and tensile strength was analyzed using response surface methodology. Experiments were planned as per central composite design and analysis of variance was performed to evaluate the significant parameters. SEBS content in the polymer solution significantly affected the shrinkage of SC‐3DP samples. Moreover, relative density and tensile strength were significantly affected by print speed and layer height. A significant interaction between print speed and layer height was also noticed for tensile strength and relative density of printed samples. Multi‐objective optimization using genetic algorithm was also performed to minimize shrinkage and maximize relative density and tensile strength. Finally, a case study was conducted comparing the physicomechanical properties of SC‐3DP samples printed at optimized process parameters and compression molded samples.Highlights Statistical models were developed using response surface methodology. Genetic algorithm based multi‐objective optimization was performed. Optimum solvent‐cast 3D printing (SC‐3DP) process parameters were determined.