Cellulose has experienced a renaissance as a precursor for carbon fibers (CFs). However, cellulose possesses intrinsic challenges as precursor substrate such as typically low carbon yield. This study examines the interplay of strategies to increase the carbonization yield of (ligno-) cellulosic fibers manufactured via a coagulation process. Using Design of Experiments, this article assesses the individual and combined effects of diammonium hydrogen phosphate (DAP), lignin, and CO2 activation on the carbonization yield and properties of cellulose-based carbon fibers. Synergistic effects are identified using the response surface methodology. This paper evidences that DAP and lignin could affect cellulose pyrolysis positively in terms of carbonization yield. Nevertheless, DAP and lignin do not have an additive effect on increasing the yield. In fact, combined DAP and lignin can affect negatively the carbonization yield within a certain composition range. Further, the thermogravimetric CO2 adsorption of the respective CFs was measured, showing relatively high values (ca. 2 mmol/g) at unsaturated pressure conditions. The CFs were microporous materials with potential applications in gas separation membranes and CO2 storage systems.