We present a system for 3D printing large-scale objects using natural biocomposite materials, which comprises a precision extruder mounted on an industrial six-axis robot. This paper highlights work on controlling process settings to print filaments of desired dimensions while constraining the operating point to a region of maximum tensile strength and minimum shrinkage. Response surface models relating the process settings to the geometric and physical properties of extruded filaments are obtained through face-centered central composite designed experiments. Unlike traditional applications of this technique that identify a fixed operating point, the models are used to uncover dimensions of filaments obtainable within the operating boundaries of our system. Process-setting predictions are then made through multi-objective optimization of the models. An interesting outcome of this study is the ability to produce filaments of different shrinkage and tensile strength properties by solely changing process settings. As a follow-up, we identify optimal lateral overlap and interlayer spacing parameters to define toolpaths to print structures. If unoptimized, the material’s anisotropic shrinkage and nonlinear compression characteristics cause severe delamination, cross-sectional tapering, and warpage. Finally, we show the linear scalability of the shrinkage model in 3D space, which allows for suitable toolpath compensation to improve the dimensional accuracy of printed artifacts. We believe this first-ever study on the parametrization of the large-scale additive manufacture technique with biocomposites will serve as reference for future sustainable developments in manufacturing.